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Article Membrane-encapsulated, moisture-desorptive passive cooling for high-performance, ultra-low- cost, and long-duration electronics thermal management Graphical abstract Highlights d Passive thermal management based on a moisture desorption-absorption process d Hygroscopic salt confined by a porous membrane to prevent leakage and corrosion d Outstanding performance/cost competitiveness compared to existing passive strategies d Device performance improved by 32.65% by equipping the strategy in a real CPU Authors Zengguang Sui, Yunren Sui, Zhixiong Ding, Haosheng Lin, Fuxiang Li, Ronggui Yang, Wei Wu Correspondence ronggui@hust.edu.cn (R.Y.), weiwu53@cityu.edu.hk (W.W.) In brief Although passive thermal management strategies have shown considerable potential to alleviate the ever-increasing energy demand for electronics cooling, they have been suffering from low efficiency and high cost. We address these critical challenges using a desorption-absorption process of moisture based on a low-cost hygroscopic salt solution confined by a membrane encapsulation method. Our strategy significantly outperforms the current passive thermal management strategies with a record-high cost effectiveness, which can be useful for various cooling applications with few technological barriers. Sui et al., 2023, Device 1, 100121 December 22, 2023 ª 2023 The Author(s). Published by Elsevier Inc. https://doi.org/10.1016/j.device.2023.100121 ll mailto:ronggui@hust.edu.cn mailto:weiwu53@cityu.edu.hk https://doi.org/10.1016/j.device.2023.100121 http://crossmark.crossref.org/dialog/?doi=10.1016/j.device.2023.100121&domain=pdf OPEN ACCESS ll Article Membrane-encapsulated, moisture-desorptive passive cooling for high-performance, ultra-low-cost, and long-duration electronics thermal management Zengguang Sui,1 Yunren Sui,1 Zhixiong Ding,1 Haosheng Lin,1 Fuxiang Li,1 Ronggui Yang,2,* and Wei Wu1,3,* 1School of Energy and Environment, City University of Hong Kong, Hong Kong 999077, China 2School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, China 3Lead contact *Correspondence: ronggui@hust.edu.cn (R.Y.), weiwu53@cityu.edu.hk (W.W.) https://doi.org/10.1016/j.device.2023.100121 THEBIGGERPICTURE With the unprecedented demand for data generation and communication, the enor- mous energy consumption for electronics cooling presents an increasingly significant environmental issue. Passive thermal management has been drawing increasing interest to reduce this rising environmental impact. However, the existing technologies need great improvements in efficiency and cost effectiveness for wider adoptions. Herein, we demonstrate a passive cooling strategy that utilizes moisture desorption from a low-cost hygroscopic salt solution to extract heat and prevent devices from overheating. Impor- tantly, it can autonomously absorb moisture from the surrounding air during off hours to recover cooling capacity. This strategy can improve the performance of a real computing device by 32.65%, exhibiting a re- cord-high cost effectiveness. This strategy provides a new method for intermittent thermal regulation, with applications including electronics, batteries, solar cells, and buildings, with few technological barriers. SUMMARY Passive thermal management strategies are one of the most promising ways to reduce energy consumption for intermittent heat dissipation. However, the existing strategies encounter tough obstacles on their way to commercialization due to their low efficiencies and high costs. Herein, we propose a passive thermal man- agement strategy that relies on moisture desorption from hygroscopic salt solutions through a protective membrane that only allows water vapor to pass through; importantly, it can spontaneously recover cooling capacity during off hours. We selected lithium bromide as a cost-effective sorbent while avoiding crystalliza- tion. Outstandingly, the strategy can provide an effective cooling capacity (DTmax = 11.5 �C) for �400 min, while the measured heat flux can reach 75 kW/m2. By employing the strategy in a real computing device, its performance is improved by 32.65% with a record-high cost effectiveness. The strategy can be useful for various applications that need intermittent thermal regulation, with few technological barriers. INTRODUCTION With the ever-increasing demands for high-performance elec- tronic and communication technologies, as well as the constant push to reduce the sizes of electronic components, the power density of electronics has continued to rise.1–5 This development leads to higher heat fluxes that are challenging to heat dissipa- tion. Poor thermal management can cause tremendous heat accumulation within electronic devices, resulting in the loss of functionality and, eventually, device failure.6,7 It is estimated that the chip performance can degrade by �10% for every 2�C rise when its operating condition exceeds 70�C–80�C.8 Hence, developing an effective thermal management strategy is essen- Device 1, 100121, Dec This is an open access article und tial for electronics.9 While active cooling technologies with forced air or liquid circulation can achieve high cooling perfor- mance, the ever-increasing energy demand for electronics cool- ing has caused an increasingly significant environmental issue.10 Also, the active cooling strategies commonly require external power sources and complex auxiliary controls, resulting in a low adaptability in the application scenarios with strict limitations on weight and space.11–14 By contrast, passive cooling strate- gies have attracted increasing interest due to their zero global- warming potential, higher compactness, and lower maintenance cost.15 Solid-liquid phase change materials (PCMs) are the most commonly used in the existing passive thermal management strategies for electronics. Studies have demonstrated that the ember 22, 2023 ª 2023 The Author(s). Published by Elsevier Inc. 1 er the CC BY license (http://creativecommons.org/licenses/by/4.0/). mailto:ronggui@hust.edu.cn mailto:weiwu53@cityu.edu.hk https://doi.org/10.1016/j.device.2023.100121 http://crossmark.crossref.org/dialog/?doi=10.1016/j.device.2023.100121&domain=pdf http://creativecommons.org/licenses/by/4.0/ Article ll OPEN ACCESS temperature rise of electronics can be suppressed for a period of time due to the fact that PCMs absorb and store the latent heat duringmelting.16–19 Despite extensive efforts in the improvement of PCMs, low phase change enthalpy (commonly lower than 200 J/gPCM) remains a fundamental limitation. 15 Additionally, their cooling efficiency will decline rapidly as the melting front is constantly away from heat sources.20,21 One of the most promising candidates for passive thermal management is the liquid-vapor phase transition of water (i.e., desorptive cooling), which is inspired by the natural process that mammals regulate their body temperature through sweat- ing.22 Strategies for developing desorptive cooling in passive thermal management are commonly based on hydrogels and metal-organic frameworks (MOFs).15,23–25 Specifically, the hygroscopic sorbents (hydrogels or MOFs) provide highly porous structures that enable high water uptake. The water stored in the sorbents can be evaporated during peak hours of electronic devices, extracting a large amount of heat to prevent the devices from overheating (i.e., desorptive cooling). During off-peak hours, the hygroscopic sorbents can autonomously absorb moisture from the surrounding atmosphere to recover their cooling capacities (i.e., self-regeneration). However, the low mass diffusion coefficients of hydrogels (�10�12– 10�11)26,27 and MOFs (�10�13–10�11)15 lead to their extremely slow regeneration rates. Generally, hydrogel-based cooling stra- tegies rely on active replenishment of water to maintain a high heat flux,26 while MOF-based cooling strategies commonly suf- fer from an irreversiblereduction in heat andmass flux due to the binders between adsorbent particles and substrates.28 Further- more, the high cost of MOFs (over 10,000 USD/kg29) also limits their large-scale applications.30 In contrast, hygroscopic inor- ganic salts, such as LiCl and LiBr, show promise in addressing these issues due to their extremely high moisture sorption capacity and low cost.31–35 These salts have been widely used in absorption cooling,36 dehumidification,37 and atmospheric water harvesting.38 Recently, researchers have impregnated hygroscopic salts into porous hydrogels to improve their water uptake and self-regeneration capability.23,26,39 However, salt- based hydrogels commonly suffer from the salting-out effect and hydrogel collapse, resulting in corrosion risks and poor moisture sorption capacities.40,41 Herein, we develop an efficient and economical passive ther- mal management strategy that uses a porous membrane to confine a low-cost hygroscopic salt into a heat sink, achieving an ultra-high equivalent enthalpy of 2,370 kJ/kg compared with the traditional PCMs. We discuss the working principle and heat/mass transfer process of the hygroscopic salt-loadedmem- brane-encapsulated heat sink (HSMHS) in detail. Two commonly used hygroscopic salts (i.e., LiCl and LiBr) are characterized and analyzed, demonstrating that LiBr is the optimal selection for this strategy. We also conduct proof-of-concept experiments to test the effects of heat flux, solution concentration, and solution layer thickness on the cooling performance. Through these experi- ments, we demonstrate that the proposed strategy is capable of offering a long-duration stable cooling capacity without solu- tion leakage and corrosion, which can suppress the temperature rise of an emulated heater with a record-high cost effectiveness compared with state-of-the-art passive cooling strategies. The 2 Device 1, 100121, December 22, 2023 cooling capacity of the strategy is further demonstrated in a cen- tral processing unit (CPU) of a real computing device, achieving an improvement of 32.65% in the device performance. Addition- ally, an analytical and finite element model is developed and vali- dated by the experimental data, which can guide further optimi- zation design. RESULTS Design and working principle of HSMHSs Figure 1A illustrates the schematic working cycle of the passive thermal management strategy. The cycle consists of desorption and absorption processes, depending on the vapor pressure difference between the salt solution (pm,s) and the surrounding atmosphere (pv), where pm,s is determined by the solution tem- perature and concentration. Figure S1 depicts the vapor partial pressure and theoretical sorption equilibrium lines of LiBr solu- tion. The reaction equilibrium equations can be found in Note S1. In a typical operating condition (i.e., 60% relative humidity [RH] and 25�C), the initial solution absorbs heat (from point a to point b), desorbing moisture from the solution to prevent the sur- face temperature of electronic devices from rising. Then, the desorption process ismaintained for a certain duration as the so- lution temperature gradually decreases due to a high pm,s (from point b to point c). Once pm,s is lower than pv, the concentrated solution spontaneously absorbs moisture from the surrounding atmosphere (from point c to point a) to recover cooling capacity. The cycle shows a fully passive desorption-absorption process, where the salt solution is confined by a porous polytetrafluoro- ethylene (PTFE) membrane that offers a vapor transfer interface while preventing solution leakage and corrosion risks. Notably, crystallization should be avoided in the desorption-ab- sorption cycle, which can deteriorate the mass and heat transfer performance. We designed and fabricated the HSMHS based on a 3D-print- ing heat sinkwith an anti-corrosion graphene coating (Figure 1B). The HSMHS consists of a hollow plate, a porous membrane, a 3D-printing heat sink, and a hygroscopic solution, and the tested prototype of the HSMHS is shown in Figure 1C. In the prototype, a 0.25-mm-thick hydrophobic membrane with a pore size of 0.45 mmwas employed (Figures 1D and S2). A schematic illustra- tion for an electronic device equipped with HSMHS is shown in Figure 1E. The HSMHS was directly attached at the electronic device. Compared to the conventional heat dissipation methods (i.e., surface convection and radiation), the desorption process of salt solution takes away a substantial part of heat generated by the electronic device, releasing water vapor to the surround- ing atmosphere through the porous membrane, and thus further preventing the device from overheating. To understand the working principle of the HSMHS, we have conducted a detailed analysis of both heat andmass transfer processes (Note S3). Fig- ure S3 depicts the simplified heat transfer process through the porous membrane. The thermal resistances, which include the external thermal resistances and the thermal resistance across the porous membrane (sm/km), play a critical role in determining the temperature difference between the solution-membrane surface and the surrounding environment. The amount of heat extracted from the solution (qcooling) can be expressed as Figure 1. Overall working principle of the proposed thermal management strategy (A) Schematic illustration of the desorption and absorption processes. In the desorption-cooling process, moisture evaporates from the solution for heat removal. In the absorption-regeneration process, the concentrated salt solution with a lower temperature absorbs moisture from the surrounding atmosphere to autonomously recover cooling capacity. The porous membrane prevents the solution leakage and device corrosion while allowing the water vapor to pass through. (B) Schematic of the fabrication process for the HSMHS. (C) Photograph of the HSMHS prototype. (D) High-magnification SEM image of the PTFE membrane with a pore size of 0.45 mm to show the nodes and fiber structures. The inset shows a photograph of the contact angle for 39.4% LiBr solution on the PTFE membrane. Details can be found in Figures S2 and S4. (E) Schematic illustration of electronic cooling with the HSMHS. Except for the common natural convection and radiation, the salt solution can extract the heat generated by the electronic de- vice, releasing water vapor through a protective membrane and thus further preventing the device from overheating. Article ll OPEN ACCESS qcooling � 1 hnat + 1 hrad + 1 hdes + sm km � = Tsurf � Tamb (Equation 1) where hnat is the natural convection heat transfer coefficient, hrad is the effective radiation heat transfer coefficient, hdes is the equiva- lent heat transfer coefficient due to the desorption process, sm is the membrane thickness, km is the thermal conductivity of the membrane, Tsurf is the temperature of solution-membrane inter- face, and Tamb is the ambient temperature. It is evident that the desorption process of salt solution extracts more heat compared with a conventional natural convection of air, thus contributing to themitigationof temperature rise inelectronicdevices.With regard to cooling capacity involved in the desorption process (qdes), it is related to thedesorptivemassflow (J) drivenby thevaporpressure difference, and qdes can be expressed as qdes = JhfgDm = Akm;m � pm;s � pv � hfgDm (Equation 2) where A is the mass transfer area; hfg is the vaporization enthalpy of water in the salt solution; km,m is the mass transfer coefficient through the porous membrane (see details in Note S3); pv is considered as an external boundary condition, which can be calculated according to the ambient condition (RH and Tamb); pm,s can be evaluated according to Figure S1; and Dm is the water content variation of the salt solution in the desorp- tion process. It can be seen from Equation 2 thatthe hygro- scopic salts used in the passive cooling strategy should feature fast desorption/absorption kinetics and high water uptake. Desorption-absorption performance for LiBr-loaded heat sinks As discussed in Figure 1, hygroscopic salts as the sorbents directly determine the cooling performance of the proposed strategy. LiCl and LiBr are themost commonly used hygroscopic salts in absorption heat storage and cooling systems,36,42 both of which have a high hygroscopic capacity and can be deli- quesced at an extremely low RH (Table S1), especially for LiBr. To test the desorption-absorption performance of the LiBr solu- tion, we built proof-of-concept prototypes (see details in Note S2). First, three LiBr solutions with mass fractions of 39.4%, 44.2%, and 49.4%were prepared to test the effect of initial water content on the cooling performance of the strategy. These solu- tionswere tested using a 3D-printing heat sink (Figure S5) coated with a 0.01-mm-thick anti-corrosion graphene coating. A polyi- mide film heater was used to emulate electronic devices, and its heat flux could be controlled by a DC power. To reduce heat loss from the bottom of the heat sink, the heat sink was placed on an insulation foam. We then placed the entire hygroscopic salt-loaded heat sink (HSHS) in an environmental chamber (Figures 2A and S6), where Tamb and RH fluctuations were kept below 1�C and 3%, respectively (Figure S7). To analyze the effect of solution layer thickness, the HSHSs with so- lution layer thicknesses of 1.0, 1.5, and 2.0 mm were prepared, respectively. During the experiments, we first removed the porous membrane to measure the desorption and absorption Device 1, 100121, December 22, 2023 3 Figure 2. Desorption and absorption experiments with a typical ambient condition (RH 60% and 25�C) (A) Schematic of the HSHS in an environmental chamber. In the chamber, the surrounding temperature and RH fluctuations can be kept below 1�C and 3%, respectively. (B) Temperature andmass evolutions of the HSHSswith different solution layer thicknesses at a heat flux of 2.41 kW/m2 (xLiBr= 39.4%). The temperature recorded by a thermocouple (TC1) shown in Figure S5 is treated as the temperature of the HSHS. For comparison, another 3D-printing heat sink was prepared as the baseline sample. (C) IR images of the HSHSs with different solution layer thicknesses. (D) Temperature evolutions at different heat fluxes. The initial solution concentration and thickness are 39.4% and 1.5 mm, respectively. (E) Performance comparison in terms of the maximum transient cooling power and temperature. Error bars are calculated depending on the propagation of instrument uncertainty. (F) Variation of thermal resistances induced by the salt solution in the desorption process. Article ll OPEN ACCESS performances of LiBr solutions, and thermocouples and high-ac- curacy mass balance were used to monitor the temperature evolution and mass change of the HSHS, respectively. Experimental data from Figure 2B show the temperature and mass evolutions of the HSHSs at a heat flux of 2.41 kW/m2. Dur- ing the initial period, using salt solution significantly slows down the temperature rise rate, resulting in a lower temperature compared with the baseline. The fast desorption process of the salt solution is responsible for this phenomenon, as confirmed by the corresponding mass curves (Figure 2B). As the heating continues, the desorption rate (i.e., desorptive mass flow shown in Equation 2) gradually decreases due to the increasing solution concentration. The temperatures of the HSHSs are fixed around the maximum values establishing quasi-stable states, achieving a lower temperature (between 58.7�C and 60.6�C) compared with the baseline (64.5�C). The temperature reductions can be ascribed to the alternate desorp- tion-absorption process (insets in Figure 2B) and enhanced heat transfer caused by a high solution concentration with a thin solu- tion layer.43,44 On the basis of the experiments, it is found that the maximum temperature difference between the HSHS and the baseline further increases as the solution layer thickness in- 4 Device 1, 100121, December 22, 2023 creases from 1.0 to 2.0 mm, with DTmax,1.0mm = 10.8 �C, DT max,1.5mm = 11.7 �C, and DT max,2.0mm = 13.0�C, respectively. Additionally, nearly the same desorption rate (green dashed line shown in Figure 2B) is observed for the three HSHSs at the initial periods, regardless of the solution layer thickness. The reason is that the water vapor transport occurs at the solution-air interface, and the desorption rate is controlled by the ambient conditions un- der a given heat flux.45 However, the HSHS (2.0 mm) can evapo- rate more water vapor than the other HSHSs (1.0 and 1.5 mm) due to its high initial water content, achieving a better cooling per- formance (Equation 2). To further understand the physical mecha- nism during the quasi-stable states, the temperature and mass curves were magnified (insets in Figure 2B). The magnified mass evolution shows an alternating process of desorption and absorp- tion, which can be attributed to a delicate balance between the heat flux and the heat dissipation by natural convection, radiation, and desorption (Equation 1). Figure 2C illustrates the temperature distribution of the baseline and the HSHSs obtained from infrared (IR) images, and a uniform temperature distribution is observed. Generally, electronic devices should operate at temperatures below 70�C Figure 2D shows the temperature evolutions of the HSHS with a 1.5-mm-thick solution layer, illustrating that the Article ll OPEN ACCESS maximum heat flux allowed is around 3.28 kW/m2 for the HSHS, corresponding to a maximum cooling power of �462.5 W/m2 (Figure S8). To understand the effect of initial water content of the salt solution on the cooling performance, we conducted a series of experiments with 39.4%, 44.2%, and 49.4% LiBr solutions. Fig- ure S9 shows the temperature and mass evolutions for the ex- periments conducted at a given heat flux of 2.41 kW/m2. As the solution concentration increases from 39.4% to 49.4% at a fixed solution layer thickness, the temperature of the quasi-sta- ble state increases due to the decreasing cooling performance. By deriving themass curves (Figure S9), the transient cooling po- wer is obtained (Figure S10). The cooling power increases with a similar tendency in the initial several minutes for the HSHSs with different solution layer thicknesses and fluctuates during quasi- stable states. The maximum cooling powers for the various HSHSs are shown in Figure 2E, with the corresponding average temperatures at quasi-stable states shown above the bars. Obviously, the HSHS with low solution concentration outper- forms other HSHSs. The maximum cooling power has a positive correlation with the solution layer thickness, especially for the HSHS with a low solution concentration. For example, by increasing the solution layer thickness from 1.0 to 2.0 mm, the maximum cooling power of the HSHS with a solution concentra- tion of 39.4%, 44.2%, and 49.4% is improved by 73.1%, 67.8%, and 54.1%, respectively. The maximum cooling power achieved is up to 409.1 W/m2 with the lowest average temperature of 58.7�C. Meanwhile, we discussed the solution concentration at the quasi-stable states (Figure S11). The solution concentration is between 57.6% and 62.6%, demonstrating that the salt solu- tion would not crystalize in the desorption processes (Figure S1). Figure 2F shows the variation of the solution thermal resistance at the starting and ending points of the desorption processes (Figure S9). The thermal resistance is linearly related to the solu- tion layer thickness. Moreover, the thermal resistance is lower at the ending points than that at the starting points due to the thin- ning solution layer thickness during desorption process. Working performance under intermittent heatgeneration To achieve a high-efficiency thermal management in some appli- cations with intermittent heat generation, it is important for HSHSs to not only have excellent cooling performance but also enable high self-regeneration capability. We conducted ex- periments at a heat flux of 2.41 kW/m2 for 10, 20, and 30 min to analyze the effect of desorption time on regeneration time (Fig- ure S12). It can be clearly seen that the desorption process continued for a period of time even after stopping heating, which can be attributed to a high pm,s caused by a high solution tem- perature. As the solution temperature further decreases, the ab- sorption process occurs when pm,s is lower than pv (Equation 2). Also, Figure S12 shows that the temperature evolutions are un- affected by the absorption process, indicating that the dilution heat caused by the absorption process is negligible in small- size HSHSs. The relationship between the desorption time and the regeneration time is depicted in Figure 3A, demonstrating that the salt solution enables self-regeneration capability. At a given desorption time, the regeneration time is decreased as the solution concentration increases from 39.4% to 49.4%, indi- cating that a high solution concentration can endow the HSHSs with rapidly self-regeneration capability, which is critical for practical applications of the proposed strategy. It is worth noting from Figures 2E and 3A that the conflict between the cooling po- wer (low solution concentration) and the regeneration time (high solution concentration) is unavoidable. Considering that the solution concentration eventually depends on the surrounding atmosphere, increasing the heat and mass transfer area can provide an effective method to reduce the regeneration time for achieving a more efficient thermal management in some application scenarios. In addition, the HSHS with a solution concentration of 39.4% (1.5-mm-thick solution layer) was tested under a periodic heat flux to discuss the effect of regeneration periods on the cooling performance. Figure 3B compares the temperature evolutions of the HSHS and the baseline (desorption, 3.28 kW/m2 for 10 min; regeneration, 0 kW/m2 for 10 min). In the initial several cycles, the cooling efficiency slightly decreases due to incom- plete solution regeneration. After several cycles, a stable cooling efficiency is achieved and the peak temperature can become nearly constant with a temperature drop of around 16.8�C. The variation of the cooling efficiency can be validated by Figure 3C, where the mass change of the desorption and absorption pro- cesses within each cycle gradually reaches an equilibrium (i.e., green column tends to 0 after several cycles). In Figure S13, we also conducted the cyclic experiments with the regeneration periods of 20 and 30 min, respectively. Results indicate that, even if the initial solution of HSHSs is in an unsaturated state (i.e., pm,s s pv), the HSHSs can still provide efficient thermal management. Figure 3D illustrates that the difference between the peak temperature of the first cycle and the peak temperature of the last cycle (i.e., black dashed boxes shown in Figure 3B) is 8.0�C, 6.5�C, and 3.6�C with the regeneration periods of 10, 20, and 30 min, respectively. Apparently, the degradation of the cooling efficiency becomes insignificant as the regeneration time increases. Notably, benefiting from the anti-corrosion char- acteristics of the graphene-based coating, no visible signs of corrosion were observed during the experiments. Cooling performance of LiBr-loaded membrane- encapsulated heat sinks Porous PTFE membranes feature vapor permeability and strong chemical stability, which play a key role to confine the salt solu- tion and achieve a long-duration stable cooling performance. An HSMHS with 5.0-mm-thick solution layer was developed to demonstrate these characteristics. The mass and temperature variations of the tested devices with and without the membrane were compared at a given heat flux of 2.41 kW/m2. From Fig- ure 4A, the mass evolutions show nearly the same tendency dur- ing the initial periods (black dash line depicted in Figure 4A), indi- cating that the mass transfer resistance caused by the membrane is insignificant. Eventually, the HSMHS shows larger mass loss compared with the strategy without the membrane, and we attribute this to the higher temperature of the HSMHS in the quasi-stable state. As shown in Figure 4B, the maximum temperature differences between the baseline and two samples (i.e., HSMHS and HSHS) are 11.5�C and 12.2�C, respectively. Device 1, 100121, December 22, 2023 5 Figure 3. Cyclic experiments of HSHSs with a typical ambient condition (RH 60% and 25�C) (A) Relation between the desorption duration and the regeneration duration at a given heat flux of 2.41 kW/m2. The regeneration duration is counted from stopping heating. Details can be found in Figure S12. (B) Cyclic stability test of the HSHS at a heat flux of 3.28 kW/m2 for 10 min, and the concentrated solution spontaneously absorbs water vapor from the sur- rounding atmosphere for 10 min. (C) Mass changes during the desorption and absorption processes within each cycle. (D) Comparison between the peak temperature of the first cycle and the peak temperature of the last cycle (black dashed boxes shown in Figure 3B) for the HSHS with different regeneration periods. Article ll OPEN ACCESS The quasi-stable temperature of the HSMHS is slightly higher than that of the HSHS, with an average temperature difference of �1.3�C. To quantitatively discuss the effect of the membrane on the duration of the thermal management, we defined an effec- tive cooling time (teff) as themoment when the temperature of the proposed strategies exceeds that of the baseline. It is found that introducing membrane reduces the effective cooling time from �520 to�400min (Figure 4B). Nevertheless, the HSMHS can still significantly extend the effective cooling time by �10-fold compared with an MOF-101(Cr)-based cooling strategy.15 Moreover, a 12 V direct-current (DC) fan was used to provide the forced airflow (Figure S14). Comparison results indicate that the forced convection affects the effective time insignifi- cantly, which can be attributed to a lower desorption tempera- ture.15 Furthermore, comparison between Figures 2B and 4B demonstrates that increasing the solution layer thickness from 1.0 to 2.0 mm enhances the cooling capacity of HSHSs; howev- er, the cooling capacity is decreased as the solution layer thick- ness increases to 5.0 mm. It suggests that an optimal solution layer thickness exists between 1.0 and 5.0 mm at the given boundary conditions. In practical applications, users can deter- 6 Device 1, 100121, December 22, 2023 mine the optimal solution layer thickness by utilizing the analyt- ical model developed in Note S3 while considering specific working conditions. Developing low-cost and high-performance cooling materials is the key for realizing the large-scale application of passive cool- ing strategies. We used an equivalent index (h) (i.e., the cooling performance per USD) to quantitate the cost effectiveness of cooling strategies, defined as h = Dmwhfg ms Cs;t (Equation 3) where Dmw represents the mass loss of water in a desorption process, ms is the mass of sorbents, and Cs,t is the cost of sor- bents. Figure 4C shows the quantitative comparison re- sults.15,17,46–55 In the comparison, the equivalent enthalpy (heq) of the selected sample is �2370 J/g (i.e., the corresponding en- ergy density [qeq] is �1.31 J/mm3) at a heat flux of 3.28 kW/m2 (corresponding to Dmw = 1.165 g and ms = 1.178 g), which is higher than existing liquid-vapor passive cooling techniques Figure 4. Cooling performance of HSMHS (A) Mass evolutions of the tested devices with and without the membrane. The inset is a photograph of the HSMHS. A 5.0-mm-thick LiBr solution with a solutionconcentration of 39.4% was employed. (B) Temperature evolutions of the tested devices with and without membrane at a heat flux of 2.41 kW/m2. A fan (12 V) was used to force ambient air to flow through the upper surface of the heat sink (Figure S14). The temperature of the HSMHS is slightly higher than that of the HSHS, indicating that introducing the membrane increases additional thermal resistance. (C) Cost effectiveness of HSMHSs compared with that of existing cooling strategies reported in the literature (see Table S3 for details). Article ll OPEN ACCESS (Table S2). The detailed price data can be found in Table S3. An improvement of about three orders of magnitude in the cost effectiveness can be achieved compared with the state-of-the- art MOF-based cooling strategies, demonstrating that the proposed cooling strategy is a promising technology toward commercialization. Thermal management for a real CPU The regeneration rate is a key parameter that measures the ther- mal management capacity of moisture-desorptive passive cool- ing strategies. To demonstrate the superiority of the proposed cooling strategy, we compared the regeneration rates of the proposed strategy with those of the existingMOF-based and hy- drogel-based cooling strategies. In Figure S15, the regeneration rate of the proposed strategy is up to 25.14 g/(m2,h), which is 1.2 times and 1.3 times that of the MOF-based and hydrogel-based cooling strategies,15,23 respectively. To further reduce the regen- eration time and improve the practicality of the proposed cooling strategy, we utilized a needle heat sink with hollow fiber mem- branes to enhance the heat and mass transfer process. The heat sink was made of aluminum to reduce weight and cost, and its physical structure can be found in Figure S16. We used an elastic PTFE hollow fiber membrane with a pore size of 0.45 mm to confine the LiBr solution (Figure S17). The hygroscop- ic salt-loaded membrane-encapsulated needle heat sink (HSMNHS) was tested at a heat flux of 2.41 kW/m2 for various RH conditions (RH 60%, RH 70%, and RH 80%), with the tem- perature and mass data recorded until the mass recovered to 0 (Figure S18). An obvious reduction in regeneration time for RH 80% is observed. This can be ascribed to the fact that the high RH accelerates the vapor absorption of the HSMNHS from the surrounding environment, as elucidated in Equation S15. In Figure 5A, we compared the mass curves of the HSMNHS with those of Figures S11A–S11C at the ambient con- dition of RH 60%, and the same desorption rate could be found due to a given heat flux of 2.41 kW/m2. The mass curve of HSMNHS rises faster than that of other samples benefiting from the improved heat and mass transfer process, and the regeneration rate of HSMNHS is improved by 335% compared to the HSHS with a solution thickness of 2.0 mm (Figure S19). Furthermore, Figure 5B compares the temperature of the HSMNHS with that of a conventional needle sink to demonstrate the outstanding thermal management capacity of the HSMNHS at the ambient condition of RH 60%. In the cyclic experiment (2.41 kW/m2 for 10 min and 0 kW/m2 for 10 min), the maximum peak-temperature difference between the HSMNHS and the conventional needle heat sink is 15.1�C, which occurs in the sec- ond cycle. The temperature difference decreases gradually and is stabilized at �8.7�C ultimately. To demonstrate the thermal management capacity of the proposed strategy at heavy loads, we applied the HSMNHS to a high-power field effect transistor (Figures S20A to S19C). Three heat sinks (i.e., needle heat sink [NHS], fin heat sink [FHS], and HSMNHS) were tested in room environment (Figures S20D to S19F), and their detailed compar- ison is listed in Table S4. Figure S21 shows the temperature and effective heat transfer coefficient evolutions for the three heat sinks at various heat fluxes (i.e., 25, 50, and 75 kW/m2). Compared to the NHS, the HSMNHS has overwhelming advan- tages in cooling performance. HSMNHS shows a competitive temperature reduction and heat transfer coefficient compared to the FHS at a given heat flux (Figures 5C and S21), even if the volume and heat transfer area of the FHS are �5 and �10 times that of the HSMNHS (Table S4), respectively. The results demonstrated that the proposed HSMNHS enables outstanding cooling performance at high heat fluxes. Notably, we did not observe any solution leakage and corrosion phenomena during the experiments. To demonstrate the cooling capacity of the improved strategy in a real scenario, we placed the HSMNHS on a CPU surface of a real computing device (ODROID-XU4). In Figure 5D, we used TCs to record the temperature of the CPU surface equipped with the HSMNHS and the original heat sink, respectively. The computing device was run on the Android system, which was driven by a professional benchmark software (AnTuTu) to Device 1, 100121, December 22, 2023 7 Figure 5. Practical application of the proposed thermal management strategy (A) Mass evolutions of different samples with the same desorption time (10 min), solution concentration (39.4%), and heat flux (2.41 kW/m2). It clearly illustrated that introducing hollow fiber membranes effectively improves the absorption-regeneration capacity. (B) Cyclic experiments of the NHS with and without the membrane (2.41 kW/m2 for 10 min and 0 kW/m2 for 10 min). (C) Comparison of temperature evolutions for the HSMNHS and FHS at heavy loads (25, 50, and 75 kW/m2). (D) Photograph of ODROID-XU4 with the HSMNHS and the original heat sink. The temperature and RH during the testing periods are shown in Figure S22. (E) Temperature evolutions of the tested devices with the two cooling strategies. A program forced the device to work at a maximum power for 15min. The insets show IR images of the tested device with the two cooling strategies at the end of the testing. (F) Transient input power evolutions of the tested devices with the two cooling strategies during testing periods. Article ll OPEN ACCESS simulate a peak workload for 15 min in a room. A maximum temperature drop of 11�C from 68.5�C to 57.5�C was achieved during the testing periods (Figure 5E). As shown in the IR images inserted in Figure 5E, the proposed thermal management strat- egy enables a lower temperature for the electronic load board. Meanwhile, we measured the input power during the experi- ments using Power-Z KT002 (Figure S23). Benefiting from the outstanding cooling capacity of our proposed strategy, the tran- sient input power of the device equipped with the HSMNHS is significantly higher than that of the device with the original heat sink during the testing periods, and an improvement of 32.65% in the average input power is achieved (Figure 5F). The experi- ments confirm the enormous potential of our proposed thermal management strategy for passive cooling. Numerical simulation and analytical model We first simulated the heat loss from the bottom of the tested de- vice using a computational fluid dynamics (CFD) tool (see details in Figure S24). The simulated temperature is consistent with the experimental data, and the heat loss is �10.4% of the total heat flux. Togainmore insights into the thermalmanagement strategy, we carried out a numerical calculation using the CFD tool based on the analyticalmodel developed inNoteS3. FigureS25demon- 8 Device 1, 100121, December 22, 2023 strates that a good agreement is found between the simulations and the experimental results, indicating that the HSHS with a solution layer thickness of 3.0 mm show an outstanding cooling performance. Also, Figure S26 displays the cross-sectional tem- perature contour over time. The solution shows an uneven tem- perature distribution in the desorption process. We ascribe this unstable behavior of the temperature to thermal convection in- side the solution. Through the experimentally validated numerical simulations, we provide guidelines for integratingthe passive cooling strategy in various thermal management applications. DISCUSSION We proposed an efficient thermal management strategy with a record-high cost effectiveness based on hygroscopic salt solu- tions and demonstrated its feasibility under heavy loads. As pre- viously discussed, LiCl is also a commonly used hygroscopic salt, which possesses higher water uptake compared to LiBr (Figures S1 and S27). Hence, we conducted an experiment to evaluate the feasibility of LiCl solution for this strategy (see more details in Note S4). An obvious crystallization during desorption cooling is observed, resulting in a non-uniform tem- perature distribution with a maximum temperature difference Article ll OPEN ACCESS of 4.8�C (Figure S28). Apparently, crystallization challenges should be taken into consideration during the selection of hygro- scopic salts for the passive thermal management strategy. To demonstrate the feasibility of the proposed cooling strategy, a comprehensive evaluation was conducted by comparing it with other emerging passive cooling technologies (MOFs and hydrogels). Five representative indexes were selected in terms of desorption performance, absorption performance, cost effec- tiveness, cycling performance, and equivalent enthalpy, as shown in Figure S29. It is found that the high cost is a major chal- lenge for MOF-based cooling strategies, while hydrogel-based cooling strategies have low cycling performance due to interior structure collapse and low absorption capacity. In contrast, hy- groscopic salts confined by porous membranes enable stable thermophysical properties and high moisture sorption capacity, which provide a promising alternative for the passive thermal management of electronics. In addition, introducing porous membranes introduces an additional thermal resistance, which can cause the cooling capacity of HSMHSs to slightly decline. It can be attributed to the low thermal conductivity of PTFE membranes. With the development of materials, some additives, such as graphene, carbon nanotubes, and silica, can be added to porous mem- branes to enhance their thermal conductivities.56 Meanwhile, we noted that a thin air layer may be generated during the desorption process, resulting in a potential reduction in heat transfer, and thus optimal structural design warrants future studies. It is also found that hygroscopic salts may leak and can lead to corrosion risk of metal devices during long-term op- erations. The leakage and corrosion risks can be avoided using membrane encapsulation techniques,57,58 graphene-based anti-corrosion coatings,59 and anti-corrosion containers.60 In summary, we proposed a passive thermal management strategy based on low-cost hygroscopic salts.We demonstrated that the strategy enabled high cooling performance without the risk of solution leakage and corrosion by introducing the porous PTFEmembrane. Benefiting from the high moisture-sorption ca- pacity of hygroscopic salts, HSMHSs enable the outstanding self-regeneration capability. Compared with the existing passive thermal management strategies, the proposed strategy shows a record-high cost effectiveness for commercialization. Further- more, we developed a detailed heat and mass transfer model validated through experiments, which could provide guidelines for further optimization. Our cooling strategy is both cost effec- tive and highly scalable, which can be useful for various cooling applications with few technological barriers. EXPERIMENTAL PROCEDURES Resource availability Lead contact Further information and requests for resources and materials should be directed to and will be fulfilled by the lead contact, Wei Wu (weiwu53@cityu. edu.hk). Materials availability This study did not generate new unique materials. Data and code availability d All data that support the findings of this study are available from the lead contact upon reasonable request. d Full experimental procedures are provided in the supplemental informa- tion. SUPPLEMENTAL INFORMATION Supplemental information can be found online at https://doi.org/10.1016/j. device.2023.100121. ACKNOWLEDGMENTS The authors gratefully acknowledge the support from the Research Grants Council of Hong Kong (project numbers CityU 11212620, CityU 11215621, CityU 11218922). R.Y. acknowledges financial support from the National Nat- ural Science Foundation of China (NSFC) under grant no. 52036002. AUTHOR CONTRIBUTIONS Z.S. and W.W. conceived the concept of this work. Z.S., Z.D., H.L., and F.L. synthesized the materials. Z.S., R.S., Z.D., H.L., and F.L. designed the exper- iments. Z.S. performed the experiments. Z.S. and R.S. developed the heat and mass transfer modeling. Z.S. wrote the original manuscript draft. Z.S., W.W., and R.Y. discussed and revised the manuscript. All authors checked the manuscript. W.W. and R.Y. directed and supervised this project. DECLARATION OF INTERESTS AUS non-provisional patent (18/183,184) related to this work has been filed by W.W., F.L., Z.S., Z.D., Y.S., C.Z., and H.L. Received: July 3, 2023 Revised: September 21, 2023 Accepted: October 3, 2023 Published: October 31, 2023 REFERENCES 1. van Erp, R., Soleimanzadeh, R., Nela, L., Kampitsis, G., and Matioli, E. (2020). 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Device 1, 100121, December 22, 2023 11 https://doi.org/10.1016/j.pecs.2013.05.004 https://doi.org/10.1016/j.pecs.2013.05.004 https://doi.org/10.1016/j.ijheatmasstransfer.2018.03.075 https://doi.org/10.1016/j.ijheatmasstransfer.2018.03.075 https://doi.org/10.1038/s41598-018-29015-3 https://doi.org/10.1016/j.ijheatmasstransfer.2019.01.084 https://doi.org/10.1016/j.scib.2022.09.014 https://doi.org/10.1038/s41467-019-10960-0 https://doi.org/10.1038/s41467-019-10960-0 https://doi.org/10.1038/s41560-018-0261-6 https://doi.org/10.1016/j.enconman.2018.10.037 https://doi.org/10.1016/j.enconman.2018.10.037 https://doi.org/10.1109/TCAPT.2008.2001973 https://doi.org/10.1021/acsami.9b06198 https://doi.org/10.1016/j.matpr.2022.01.178 https://doi.org/10.1016/j.matpr.2022.01.178 https://doi.org/10.1016/j.ijheatmasstransfer.2021.122257https://doi.org/10.1016/j.ijheatmasstransfer.2021.122257 https://doi.org/10.1016/j.ijheatmasstransfer.2022.123651 https://doi.org/10.1007/s40820-021-00702-7 https://doi.org/10.1002/pat.6010 https://doi.org/10.1002/pat.6010 https://doi.org/10.1016/j.xcrp.2021.100664 https://doi.org/10.1016/j.xcrp.2021.100664 https://doi.org/10.1016/j.xcrp.2022.100879 https://doi.org/10.1016/j.cej.2019.05.034 https://doi.org/10.1016/j.xcrp.2021.100568 https://doi.org/10.1016/j.xcrp.2021.100568 Membrane-encapsulated, moisture-desorptive passive cooling for high-performance, ultra-low-cost, and long-duration electron ... Introduction Results Design and working principle of HSMHSs Desorption-absorption performance for LiBr-loaded heat sinks Working performance under intermittent heat generation Cooling performance of LiBr-loaded membrane-encapsulated heat sinks Thermal management for a real CPU Numerical simulation and analytical model Discussion Experimental procedures Resource availability Lead contact Materials availability Data and code availability Supplemental information Acknowledgments Author contributions Declaration of interests References
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