Yangliu Shi, Haoran Quan, Chuang Liu, Yue Han, Heyang Zhang, Chen Chen, He Dong, Jintao Wang, Jin Wang
{"title":"NiOx Films under Ambient Humidity Regulation: New Strategies to Enhance the Performance of Perovskite Solar Cells","authors":"Yangliu Shi, Haoran Quan, Chuang Liu, Yue Han, Heyang Zhang, Chen Chen, He Dong, Jintao Wang, Jin Wang","doi":"10.1021/acsami.5c07790","DOIUrl":"https://doi.org/10.1021/acsami.5c07790","url":null,"abstract":"Metal halide perovskite materials are highly favored in solar cells owing to their excellent power conversion efficiency, simple preparation process, and low-cost manufacturing. Among the many hole transport materials, inorganic materials are favored because of their remarkable cost effectiveness, chemical stability, and long-term stability. Although NiO<sub><i>x</i></sub> is preferred in inorganic hole transport layer material due to its excellent performance, its high reactivity with the perovskite interface may lead to interface defects and carrier recombination, affecting the long-term stability of the device. To further enhance both the performance and long-term stability of perovskite solar cells, the effect of environmental relative humidity on the performance of NiO<sub><i>x</i></sub> films was discussed in this study. By comparing and analyzing the surface morphology and physical properties of NiO<sub><i>x</i></sub> films prepared under different humidity conditions, we found that relative humidity has a significant effect on the performance of NiO<sub><i>x</i></sub> films and their prepared perovskite solar cells. In particular, NiO<sub><i>x</i></sub> films prepared at 60% relative humidity and fabricated into perovskite solar cells exhibited a significantly higher short-circuit current density (<i>J</i><sub>sc</sub>) and fill factor (FF). These findings provide an important reference for optimizing the preparation process and enhancing the performance of perovskite-based solar devices.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"32 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Binder-Free Metal–Organic Framework Ion Osmosis Membrane for Stabilizing a Zn Anode","authors":"Lvgen Shen, Cheng Wang, Xinyi Du, Xiujing Lin, Ruiqing Liu, Xiaomiao Feng","doi":"10.1021/acsami.5c05136","DOIUrl":"https://doi.org/10.1021/acsami.5c05136","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) have attracted considerable attention due to their low cost and high safety. However, their development is hindered by dendrite formation and complex anodic side reactions. In this study, a binder-free zirconium-based metal–organic framework (MOF) membrane, NUS-8, is proposed as an artificial solid electrolyte interphase (ASEI) for the Zn anode, with the aim to regulate Zn<sup>2+</sup> desolvation and deposition processes, inhibit dendrite growth, and mitigate anodic side reactions. The microporous structure and abundant functional groups (–COOH, –OH) in the NUS-8 membrane enable ion flux control through an ion-confinement effect, reducing ion transfer resistance and providing stable pathways for Zn<sup>2+</sup> migration. These characteristics enhance the hydrophilicity of the Zn anode surface, accelerate the desolvation process, and lower the activation energy barrier for Zn<sup>2+</sup> migration from 28.73 to 26.10 kJ mol<sup>–1</sup>. As a result, symmetric cells with NUS-8@Zn anodes exhibited a prolonged lifespan exceeding 1180 h at 1 mA cm<sup>–2</sup> and 1 mAh cm<sup>–2</sup>, significantly outperforming bare Zn anodes (90 h). Additionally, the NUS-8@Zn||MnO<sub>2</sub> full cell demonstrated excellent cycling stability, with a capacity retention of 72.3% over 3000 cycles at 5 A g<sup>–1</sup>. This work presents a promising strategy to enhance Zn anode performance and introduces a design approach for advancing AZIBs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"51 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218949","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jan Paštika, Deniz Güngen, Amutha Subramani, Vlastimil Mazánek, Marco Serra, Lunjie Zeng, Eva Olsson, Rui Gusmão, Zdeněk Sofer
{"title":"Toward 2D van der Waals Entropy Mixture MX2 (M = Mo, W; X = S, Se, Te) for Hydrogen Evolution Electrocatalysis","authors":"Jan Paštika, Deniz Güngen, Amutha Subramani, Vlastimil Mazánek, Marco Serra, Lunjie Zeng, Eva Olsson, Rui Gusmão, Zdeněk Sofer","doi":"10.1021/acsami.5c05482","DOIUrl":"https://doi.org/10.1021/acsami.5c05482","url":null,"abstract":"High-entropy alloys have emerged as a class of materials, offering unique properties due to their irregular and randomized arrangement of multiple elements in an ordered lattice. This concept has been extended to two-dimensional (2D) van der Waals materials, including transition metal dichalcogenides (TMD), which exhibit promising applications in electrocatalysis. In this work, we have explored the synthesis of entropy mixture crystals (TMD<sub>mix</sub>) involving the chemical vapor transport of five individual elements, Mo and W as metal elements, S, Se, and Te as chalcogenide elements, resulting in a crystalline structure with a controlled composition Mo<sub>0.56</sub>W<sub>0.44</sub>(S<sub>0.33</sub>Se<sub>0.35</sub>Te<sub>0.32</sub>)<sub>2</sub>, with an estimated Δ<i>S</i><sub>mix</sub> of 0.96<i>R</i>. When observed along the [001] zone axis, STEM HAADF images indicate the presence of the different crystal phases of the 2D TMDs (1T, 2H, and 3R). Our findings demonstrate the potential of the entropy TMD<sub>mix</sub> materials as catalysts for the hydrogen evolution reaction, offering an alternative to noble metal-based catalysts. To maximize the potential of TMD<sub>mix</sub>, we chose chemical exfoliation with the resulting material being subdivided into size groups, big and small, according to their lateral size. In an acidic medium, the lowest overpotential of 127 mV and a Tafel slope of 79 mV/dec were obtained for the exfoliated sample with a small lateral size (exf-TMD<sub>small</sub>).","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"102 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218950","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lei Yang, Yun-Zhe Zheng, Abliz Mattursun, Ya-Qiong Wang, Zhao Guan, Rong Huang, Yan Cheng, Bin-Bin Chen, Ping-Hua Xiang, Chun-Gang Duan, Ni Zhong
{"title":"Unconventional Thermal Stability of Domain Framework in Ferroelectric CuInP2S6","authors":"Lei Yang, Yun-Zhe Zheng, Abliz Mattursun, Ya-Qiong Wang, Zhao Guan, Rong Huang, Yan Cheng, Bin-Bin Chen, Ping-Hua Xiang, Chun-Gang Duan, Ni Zhong","doi":"10.1021/acsami.5c04037","DOIUrl":"https://doi.org/10.1021/acsami.5c04037","url":null,"abstract":"Achieving stable and persistent polarization characteristics in ferroelectric (FE) materials is crucial for fabricating high-density, low-power multifunctional memories. In this study, we conducted a comprehensive investigation of the 2D FE material CuInP<sub>2</sub>S<sub>6</sub> (CIPS), employing piezoelectric force microscopy (PFM), scanning transmission electron microscopy (STEM), and Raman spectroscopy. By comparing CIPS with and without the nonferroelectric (NFE) phase, we observed unexpected stability of the domain framework at high temperatures. This was evidenced by in situ temperature-dependent PFM measurements and Raman spectra. STEM analysis revealed Cu ion defects and charge accumulation at the FE/NFE interface, which contributed to the thermal stability due to a strong pinning effect. This work highlights the significant positive impact of NFE phases on the thermal stability of FE CIPS, providing insights into the development of controllable FE polarization switching and the potential application of highly reliable and durable multifunctional devices.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"52 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Enhanced and Tunable Emission from Organic–Inorganic Metal Halide Perovskites A2ZrCl6:Sb3+ via A-Site Organic Cation Manipulation","authors":"Ming-Xiang You, Zeyu Lyu, Qingxian Xu, Dashuai Sun, Taixing Tan, Pengcheng Luo, Zheng Lu, Hongpeng You","doi":"10.1021/acsami.5c03942","DOIUrl":"https://doi.org/10.1021/acsami.5c03942","url":null,"abstract":"The substitution of an inorganic cation (such as Cs<sup>+</sup>) by an organic group has provided a great opportunity for enhancing and enriching the emission from metal halide perovskites because of the abundant changes in the organic molecule. However, the emission modulation by changing the organic group has been rarely reported. Herein, Cs<sup>+</sup> in Cs<sub>2</sub>ZrCl<sub>6</sub>:Sb<sup>3+</sup> was substituted by a series of organic groups. The substitution by butyltriphenylphosphonium (BTP) generated a monoclinic crystal with a <i>P</i>2<sub>1</sub>/<i>n</i> space group, which was determined by single-crystal diffraction. (BTP)<sub>2</sub>ZrCl<sub>6</sub>:Sb<sup>3+</sup> features typical dual-band emissions from self-trapped excitons. Moreover, because of the large distance (>11 Å) among the [ZrCl<sub>6</sub>]<sup>2–</sup> octahedra, more Sb<sup>3+</sup> dopants can be tolerated before concentration quenching. Consequently, (BTP)<sub>2</sub>ZrCl<sub>6</sub>:Sb<sup>3+</sup> exhibited high inner and external quantum efficiencies of 96.2 and 73.5%, respectively. Furthermore, the butyl group of BTP was changed to other groups with different sizes and electronic states. The small change of the organic group can effectively tailor the emission intensity (<i>I</i><sub>maximum</sub>/<i>I</i><sub>minimum</sub> = 7.06 ± 0.08) and wavelength (615–665 nm). The applications of (BTP)<sub>2</sub>ZrCl<sub>6</sub>:Sb<sup>3+</sup> in white light-emitting diodes (WLEDs) and anticounterfeiting were demonstrated. Our work not only presents well-performed organic–inorganic metal halide perovskites but also indicates the need for an elaborate design of the organic cations.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"62 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211669","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hua Yan, Chunfei Dai, Xingkun Luan, Hang Li, Chen Wang, Xiaona Li, Xuezhong Du
{"title":"Near-Infrared Light-Responsive Upconversion Nanoparticles Supported Elemental Selenium for Combination Tumor Therapy: Selenium Therapy, Photocatalytic Therapy, and “AND” Logic-Gated Chemotherapy","authors":"Hua Yan, Chunfei Dai, Xingkun Luan, Hang Li, Chen Wang, Xiaona Li, Xuezhong Du","doi":"10.1021/acsami.5c08003","DOIUrl":"https://doi.org/10.1021/acsami.5c08003","url":null,"abstract":"Multimodal tumor therapy based on “all-in-one” nanoplatforms enhances therapeutic efficacy, simplifies the construction process, and improves material utilization. Elemental selenium was successfully supported on upconversion nanoparticles (UCNPs) to constitute the near-infrared (NIR) light-responsive UCNP@Se heterostructures for the first time. Under 980 nm irradiation, the UCNP@Se heterostructures could not only produce holes and superoxide radicals •O<sub>2</sub><sup>–</sup> but also catalyze the generation of hydroxyl radicals •OH by highly elevated levels of H<sub>2</sub>O<sub>2</sub> in tumor cells to kill the tumor cells. In addition to the superior photocatalytic performance, elemental selenium itself also exhibited inherent inhibition activity against tumor cells. On the basis of the binding of anthracycline anticancer drugs such as doxorubicin (DOX) to the supported elemental selenium through Cu<sup>2+</sup> bridging coordination, the UCNP@Se–Cu-DOX drug delivery system was constructed. The introduction of Cu<sup>2+</sup> not only improved the efficient loading of DOX but also achieved the “AND” logic-controlled release of DOX under the combined stimuli of low pH and overexpressed glutathione (GSH) in tumor cells. Moreover, the loaded Cu<sup>2+</sup> reacted with the overexpressed GSH to generate the active species Cu<sup>II</sup>-GSSG upon NIR light irradiation, which further promoted tumor cell apoptosis. The NIR light-responsive UCNP@Se–Cu-DOX drug delivery system achieved the combination tumor therapy of selenium therapy, photocatalytic therapy, and logic-gated chemotherapy and has great potential applications in tumor therapy.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"135 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218955","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xi Guo, Junwei Zeng, Jijun Yun, Pengxiang Zhao, Yuhan Chang, Wenjie Song, Yalu Zuo, Guoqiang Yu, Hao Wu, Li Xi, Baoshan Cui
{"title":"Topological Insulators Boost Ultralow-Power Neuromorphic Spintronics: Advancing Handwritten Digit Recognition with High SOT Efficiency","authors":"Xi Guo, Junwei Zeng, Jijun Yun, Pengxiang Zhao, Yuhan Chang, Wenjie Song, Yalu Zuo, Guoqiang Yu, Hao Wu, Li Xi, Baoshan Cui","doi":"10.1021/acsami.5c04885","DOIUrl":"https://doi.org/10.1021/acsami.5c04885","url":null,"abstract":"Neuromorphic spintronics devices driven by spin–orbit torque (SOT) offer advantages in integration density, durability, and scalability for high-performance artificial intelligence systems. However, the development of ultralow-power neuromorphic computing is hindered by the low SOT efficiency (<i>θ</i><sub>SH</sub> < 1) in conventional heavy metals. In this work, we demonstrate low-power artificial synapses and neuron devices that simultaneously achieve long-term potentiation/depression and excitatory/inhibitory postsynaptic potential processes with an ultralow activation current density of 1.8 × 10<sup>5</sup> A/cm<sup>2</sup>, which is 1–2 orders of magnitude lower than that in traditional heavy metal systems, owing to the exceptional SOT efficiency of (BiSb)<sub>2</sub>Te<sub>3</sub> (<i>θ</i><sub>SH</sub> = 1.11). Furthermore, an artificial neural network utilizing our low-power synapses and neurons achieved 92.8% accuracy in handwritten digit recognition, highlighting topological insulators as promising candidates for low-power neuromorphic spintronics.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"56 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144219012","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Triet Thien Huu Nguyen, Jiawen Ren, Billy James Murdoch, Josh Lipton-Duffin, Jennifer M Macleod, Daniel E Gómez, Joel van Embden, Enrico Della Gaspera
{"title":"Doping and Annealing Conditions Strongly Influence the Water Oxidation Performance of Hematite Photoanodes.","authors":"Triet Thien Huu Nguyen, Jiawen Ren, Billy James Murdoch, Josh Lipton-Duffin, Jennifer M Macleod, Daniel E Gómez, Joel van Embden, Enrico Della Gaspera","doi":"10.1021/acsami.5c05059","DOIUrl":"10.1021/acsami.5c05059","url":null,"abstract":"<p><p>Hematite (α-Fe<sub>2</sub>O<sub>3</sub>) is one of the most promising semiconductors for solar water splitting due to its high theoretical efficiency and low cost. However, its poor electronic properties strongly limit its performance. Furthermore, the impact of composition and processing conditions on such properties, and on the water splitting efficiency, is poorly understood. Here, we unravel the role of these contributions and provide guidelines for the fabrication of efficient hematite photoanodes. Aliovalent doping with tin and fluorine is found to improve the electrical conductivity of hematite, leading to higher performance. Annealing in an inert atmosphere, which is conventionally used to create oxygen vacancies, is found not to affect undoped hematite. However, a marked effect has been observed in doped hematite, and a model describing dopant activation rather than oxygen vacancy formation has been proposed. The synergy between the presence of both dopants and the annealing conditions provides optimal electrical properties, which enable the increase of the hematite thickness, leading to enhanced light absorption and limiting the detrimental charge recombination issues observed in undoped films or even in doped films processed in excess oxygen. Our work provides a deeper understanding of the interplay among all of these processing factors, resulting in hematite photoanodes with increased performance.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"32635-32645"},"PeriodicalIF":8.3,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144126118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Multifunctional-Ligand Enabled Stable CsPbI3 Quantum Dots for Highly Efficient Pure-Red Light-Emitting Diodes","authors":"Shuwen Huang, Xiaoming Mo, Shulin Han, Huasong Liang, Lei Cai, Sheng Cao, Bingsuo Zou, Jinju Zheng, Jialong Zhao","doi":"10.1021/acsami.5c04454","DOIUrl":"https://doi.org/10.1021/acsami.5c04454","url":null,"abstract":"High-performance pure-red perovskite light-emitting diodes (PeLEDs) are promising candidates for optoelectronic applications due to their remarkable photophysical properties. However, the unstable surface and insulating long-chain capping ligands of perovskite quantum dots (QDs) pose challenges to their commercialization by compromising stability and performance. Here, a simple but effective approach was demonstrated to synthesize highly stable red CsPbI<sub>3</sub> QDs by introducing a multifunctional molecule, phenformin hydrochloride (PhenHCl), as an additive ligand. While the biguanide functional group in PhenHCl formed multiple hydrogen-bond interactions with the lead halide octahedron, the excess Cl<sup>–</sup> anions compensated for the iodine vacancies and eliminated trap states in the CsPbI<sub>3</sub> QDs. The synergistic effect of the biguanide functional group and halogen compensation significantly passivated surface defects of the red CsPbI<sub>3</sub> QDs, yielding a photoluminescence (PL) quantum yield of 98.6% and excellent ambient stability with 90% PL intensity retention over 80 days. The resulting pure-red PeLEDs based on the PhenHCl-treated CsPbI<sub>3</sub> QDs were demonstrated to show a remarkable enhancement in the electroluminescence performance at around 649 nm, with an external quantum efficiency of 13.38%, and a maximum luminance of 2159 cd m<sup>–2</sup>. Our findings in this work provide an avenue by modulating the surface chemistry of CsPbI<sub>3</sub> QDs to enhance the performance of pure-red PeLEDs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"37 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144201421","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiayi Song, Zhiheng Zheng, Shiliang Zhou, Tao Shi, Huan Liu, Xiaodong Wang
{"title":"Phase-Change Microcapsules Boosting Clean Water Production and Electricity Output through Janus Bilayer Poly(vinyl alcohol)/Chitosan Composite Aerogels","authors":"Jiayi Song, Zhiheng Zheng, Shiliang Zhou, Tao Shi, Huan Liu, Xiaodong Wang","doi":"10.1021/acsami.5c03806","DOIUrl":"https://doi.org/10.1021/acsami.5c03806","url":null,"abstract":"To address two critical global challenges─clean water scarcity and energy poverty─an innovative Janus bilayer composite aerogel is designed as a single solar-driven platform for sustainable clean water production and electricity generation. This type of Janus bilayer aerogel was successfully fabricated with a hydrophobic upper layer comprising a poly(vinyl alcohol) (PVA)/chitosan (CS)/carbon black (CB) composite aerogel and a hydrophilic lower layer based on a PVA/CS/phase-change microcapsule composite aerogel. With such a Janus bilayer structure, the composite aerogel demonstrates efficient light absorption and superior salt-resistant performance by its upper layer and prominent latent heat-storage and water-transport abilities by its lower layer. More importantly, the introduction of phase-change microcapsules enables the lower layer of the developed bilayer aerogel to store photothermal energy absorbed by its upper layer, continually driving interfacial evaporation under insufficient solar irradiation conditions. Benefiting from these advantages, the developed composite aerogel-based evaporator shows a high evaporation rate of 2.23 kg m<sup>–2</sup> h<sup>–1</sup> under one-sun irradiation alone with good resistance to salt accumulation. Compared to a control evaporator without any phase-change microcapsules, the developed evaporator obtained an increase in the total mass change of 150% under dark conditions. Meanwhile, a thermoelectrical generator equipped with the composite aerogel exhibits an open-circuit voltage of 143.89 mV under one-sun irradiation alone with an elongated power output period of 30 min. With an innovative Janus bilayer structural design by combining a biodegradable PVA/CS aerogel with phase-change microcapsules and CB nanoparticles, this study represents a significant advancement in renewable energy utilization, particularly in sustainable water purification and hybrid energy systems. The developed Janus bilayer composite aerogel exhibits great application potential in highly efficient freshwater production and electricity generation under intermittent sunlight irradiation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"52 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211674","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}