ACS Applied Energy Materials最新文献

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Dual-Dimensional Interwoven Proton Exchange Membrane Exhibiting High Anhydrous Proton Conductivity Around Room Temperature 室温下具有高无水质子导电性的二维交织质子交换膜
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-27 DOI: 10.1021/acsaem.5c02185
Nian-Yu Zhao, An-Rui Gu, Han Zhang, Xue-Wei Pan, Dong-Sheng Shao, Zheng-Fang Tian, Qiao Qiao, Jin Zhang* and Xiao-Ming Ren*, 
{"title":"Dual-Dimensional Interwoven Proton Exchange Membrane Exhibiting High Anhydrous Proton Conductivity Around Room Temperature","authors":"Nian-Yu Zhao,&nbsp;An-Rui Gu,&nbsp;Han Zhang,&nbsp;Xue-Wei Pan,&nbsp;Dong-Sheng Shao,&nbsp;Zheng-Fang Tian,&nbsp;Qiao Qiao,&nbsp;Jin Zhang* and Xiao-Ming Ren*,&nbsp;","doi":"10.1021/acsaem.5c02185","DOIUrl":"https://doi.org/10.1021/acsaem.5c02185","url":null,"abstract":"<p >Developing proton exchange membranes (PEMs) that operate efficiently around room temperature and anhydrous conditions remains a critical challenge in electrochemical devices. Conventional linear polymers typically suffer from poor confinement of strong acids and ill-defined proton conduction pathways, which limit their practical applications. Herein, we report an anhydrous proton exchange membrane (MSA@CTF-AP), which is constructed by confining a strong acid (methanesulfonic acid, MSA) within a polymeric network that consists of three-dimensional (3D) triazine frameworks interwoven with one-dimensional (1D) polymer segments. In this hybrid architecture, the rigid 3D domains provide more stable proton conduction pathways, while flexible 1D polymer segments maintain the mechanical integrity of membrane. As a result, the membrane exhibits a high anhydrous proton conductivity exceeding 10<sup>–3</sup> S cm<sup>–1</sup> around room temperature, along with excellent long-term cycling stability, retaining over 99% of its initial capacity after 7500 cycles in proton battery systems. Compared to liquid and powder-based proton electrolytes, this continuous self-standing membrane displays enhanced structural and performance stability, making it a promising proton electrolyte candidate for next-generation proton batteries and other related nonaqueous electrochemical devices operating around room temperature.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12960–12968"},"PeriodicalIF":5.5,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007395","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic Bulk-to-Surface Modification of Ni-Rich Cathodes for High-Performance Lithium-Ion Batteries 高性能锂离子电池用富镍阴极体-表面协同改性研究
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-26 DOI: 10.1021/acsaem.5c01676
Mengyao Xu, Chengxin Zhu, Jinkai Qiu, Cheng Lian, Jingkun Li, Haiping Su* and Honglai Liu, 
{"title":"Synergistic Bulk-to-Surface Modification of Ni-Rich Cathodes for High-Performance Lithium-Ion Batteries","authors":"Mengyao Xu,&nbsp;Chengxin Zhu,&nbsp;Jinkai Qiu,&nbsp;Cheng Lian,&nbsp;Jingkun Li,&nbsp;Haiping Su* and Honglai Liu,&nbsp;","doi":"10.1021/acsaem.5c01676","DOIUrl":"https://doi.org/10.1021/acsaem.5c01676","url":null,"abstract":"<p >Ni-rich layered cathodes are key materials for next-generation lithium-ion batteries (LIBs) aiming for a higher energy density and lower cost. However, their bulk and interface structural instability significantly impair their electrochemical performance, hindering their widespread application. Herein, we report a bulk-to-surface modification strategy for Ni-rich cathodes by Ti doping and Gd<sub>2</sub>O<sub>3</sub> surface coating (NCMT@Gd<sub>2</sub>O<sub>3</sub>). In this work, Ti doping and Gd<sub>2</sub>O<sub>3</sub> coating synergistically suppress cation mixing, lattice oxygen loss, and surface side reactions, thereby enhancing the structural and electrochemical stability, particularly under high-voltage operation (≥4.5 V). As a result, the NCMT@Gd<sub>2</sub>O<sub>3</sub> cathode demonstrates excellent electrochemical performance with a high discharge capacity of 194.14 mAh g<sup>–1</sup> and a high capacity retention ratio of 89.69% after 100 cycles (1C, cutoff voltage of 4.5 V). This work paves the way for the development of next-generation high-energy-density LIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12673–12683"},"PeriodicalIF":5.5,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007455","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Simultaneous Enhancement of Density of States and Phonon Scattering for Excellent Performance of Cu2SnSe3 态密度和声子散射同时增强对Cu2SnSe3优异性能的影响
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-26 DOI: 10.1021/acsaem.5c01753
Chen Zhu*, Ziqi Zhu, Kunqi Shang, Wenbin Gong, Guoxian Zhang, Lingchang Wang, Xiaosong Liu, Shijing Sang, Fali Chong* and Hongwei Ming*, 
{"title":"Simultaneous Enhancement of Density of States and Phonon Scattering for Excellent Performance of Cu2SnSe3","authors":"Chen Zhu*,&nbsp;Ziqi Zhu,&nbsp;Kunqi Shang,&nbsp;Wenbin Gong,&nbsp;Guoxian Zhang,&nbsp;Lingchang Wang,&nbsp;Xiaosong Liu,&nbsp;Shijing Sang,&nbsp;Fali Chong* and Hongwei Ming*,&nbsp;","doi":"10.1021/acsaem.5c01753","DOIUrl":"https://doi.org/10.1021/acsaem.5c01753","url":null,"abstract":"<p >As an environmentally friendly thermoelectric material, Cu<sub>2</sub>SnSe<sub>3</sub> has drawn much attention. However, the thermoelectric conversion efficiency of Cu<sub>2</sub>SnSe<sub>3</sub> is still too low to satisfy wide applications due to the high electrical resistivity ρ and low thermopower <i>S</i>. Herein, we show that around a 7-fold drop of electrical resistivity and 2.5-fold increase in thermopower (at room temperature) were simultaneously achieved by doping Co at Sn sites due to the increased hole concentration and enhanced density of states (DOS), enabling a dramatic power factor boost. Consequently, PF = 8.7 μW cm<sup>–1</sup> K<sup>–2</sup> was achieved at 848 K for Cu<sub>2</sub>Sn<sub>0.92</sub>Co<sub>0.08</sub>Se<sub>3</sub>. Moreover, both the substitution of Cu with Yb and the formation of Cu vacancies caused by Yb doping can lead to further enhancement of DOS, which gives a 1.5 times increase in <i>S</i>. In addition, as large as a 31% reduction (at 300 K) of lattice thermal conductivity was obtained because of the enhanced phonon scattering by point defects (Co<sub>Sn</sub><sup>–</sup>, Yb<sub>Cu</sub><sup>2+</sup>, and V<sub>Cu</sub><sup>–</sup>) and Yb<sub>2</sub>Se<sub>2</sub>O nanoprecipitates. As a result, a high ZT = 1.23 was achieved at 848 K for the Cu<sub>1.94</sub>Yb<sub>0.06</sub>Sn<sub>0.92</sub>Co<sub>0.08</sub>Se<sub>3</sub> sample, which is about 2.5 times larger than that of the pristine sample.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12712–12721"},"PeriodicalIF":5.5,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007459","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Harnessing Visible Light: Unraveling the Photocatalytic Water Splitting Activity of Ir–TiO2 利用可见光:揭示Ir-TiO2光催化水分解活性
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-26 DOI: 10.1021/acsaem.5c01776
Moses D. Ashie, Chandra M. Adhikari, Gayani Pathiraja and Bishnu Prasad Bastakoti*, 
{"title":"Harnessing Visible Light: Unraveling the Photocatalytic Water Splitting Activity of Ir–TiO2","authors":"Moses D. Ashie,&nbsp;Chandra M. Adhikari,&nbsp;Gayani Pathiraja and Bishnu Prasad Bastakoti*,&nbsp;","doi":"10.1021/acsaem.5c01776","DOIUrl":"https://doi.org/10.1021/acsaem.5c01776","url":null,"abstract":"<p >The quest to enhance the photocatalytic properties of TiO<sub>2</sub> for hydrogen evolution in the visible region has necessitated its modification through various strategies. In this study, a one-pot solvothermally synthesized iridium-decorated titanium dioxide (Ir–TiO<sub>2</sub>) exhibits enhanced photochemical properties for splitting water in visible light. By varying the amount of Ir precursors, Ir-doped TiO<sub>2</sub> and IrO<sub>2</sub> composites with TiO<sub>2</sub> were formed. Density functional theory (DFT) calculations reveal that Ir has localized d and f orbitals and that its oxide exhibits metallic character. When Ir replaces Ti as the dopant, energy levels appear near the Fermi level. At lower Ir concentrations, Ti still dominates, and Ti 3d hybridizes with Ir 5d, while O 2p interacts with Ir 5p, contributing to the narrowing of the band gap and modification of the chemical and electronic properties of TiO<sub>2</sub>. Photocatalytic hydrogen evolution experimental results revealed that Ir–TiO<sub>2</sub> exhibits high activity with a yield of 1636.7 μmol h<sup>–1</sup> g<sup>–1</sup> compared to pristine (238.0 μmol h<sup>–1</sup> g<sup>–1</sup>) and commercial (241.0 μmol h<sup>–1</sup> g<sup>–1</sup>) TiO<sub>2</sub>. This can be attributed collectively to the reduction of the band gap for effective light absorption, a high surface area, and efficient charge transfer. The excellent recyclability and reusability of our materials demonstrate their long-term applicability as catalysts.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12733–12740"},"PeriodicalIF":5.5,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsaem.5c01776","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007482","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Modulation of Surface Structure and Electronic States of Defective Pd-Doped NiFe-Layered Double Hydroxide Bifunctional Electrocatalyst by Alkaline Etching for Zn–Air Batteries 碱性蚀刻法调制锌空气电池用缺陷掺钯镍层双氢氧化物双功能电催化剂的表面结构和电子态
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-26 DOI: 10.1021/acsaem.5c02043
Beibei Wang, Youyuan Zhang, Dajun Wu, Fanya Jin, Zhenzhong Yang*, Shaohui Xu*, Dayuan Xiong, Lianwei Wang and Paul K. Chu, 
{"title":"Modulation of Surface Structure and Electronic States of Defective Pd-Doped NiFe-Layered Double Hydroxide Bifunctional Electrocatalyst by Alkaline Etching for Zn–Air Batteries","authors":"Beibei Wang,&nbsp;Youyuan Zhang,&nbsp;Dajun Wu,&nbsp;Fanya Jin,&nbsp;Zhenzhong Yang*,&nbsp;Shaohui Xu*,&nbsp;Dayuan Xiong,&nbsp;Lianwei Wang and Paul K. Chu,&nbsp;","doi":"10.1021/acsaem.5c02043","DOIUrl":"https://doi.org/10.1021/acsaem.5c02043","url":null,"abstract":"<p >Surface structure and electronic states are important parameters for bifunctional catalysts, especially in energy devices. Herein, the hierarchically porous defective Pd-doped NiFe-layered double hydroxide is prepared by electrodeposition and alkaline etching. The etching process increases the surface area to facilitate bifunctional catalysis of the oxygen reduction reaction/oxygen evolution reaction in Zn–air batteries (ZABs). Electrochemical assessment reveals inhibited oxidation of nickel hydroxide after alkaline etching and formation of the hybrid battery composed of Zn–Ni and ZABs, which shows high reversibility and stability. The results reveal an effective strategy to modulate the surface properties of bifunctional catalysts.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12857–12867"},"PeriodicalIF":5.5,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhanced Thermoelectric Performance from Li2SrSiS4 to Li2PbSiS4 Driven by Band Degeneracy and Antibonding-Induced Ultralow Thermal Conductivity 由能带简并和反键诱导的超低导热驱动的Li2SrSiS4到Li2PbSiS4的热电性能增强
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-26 DOI: 10.1021/acsaem.5c01780
Subhajit Sau,  and , Kanchana Venkatakrishnan*, 
{"title":"Enhanced Thermoelectric Performance from Li2SrSiS4 to Li2PbSiS4 Driven by Band Degeneracy and Antibonding-Induced Ultralow Thermal Conductivity","authors":"Subhajit Sau,&nbsp; and ,&nbsp;Kanchana Venkatakrishnan*,&nbsp;","doi":"10.1021/acsaem.5c01780","DOIUrl":"https://doi.org/10.1021/acsaem.5c01780","url":null,"abstract":"<p >Thermoelectric (TE) materials with effective energy conversion properties are essential for tackling energy crises and combating environmental challenges. Quaternary materials have recently emerged as candidates for TE applications due to their high performance. Here, we study the electronic and thermal transport properties of two tetragonal quaternary thiosilicates, Li<sub>2</sub>PbSiS<sub>4</sub> (LPSS) and Li<sub>2</sub>SrSiS<sub>4</sub> (LSSS), using first-principles calculations and Boltzmann transport theory. LPSS, a wide band gap semiconductor, is predicted to exhibit a figure of merit (ZT) of (n-type) 3.06 at 900 K, exceeding that of LSSS (n-type, 0.51) by over 6-fold. Notably, LPSS also achieves a comparable ZT for p-type (2.51) carriers, underscoring its potential for TE device applications requiring balanced n- and p-type performance. This high-performance behavior originates from the synergistic effect of multiple band degeneracy and band dispersion, resulting in an improved power factor. At 300 K, LPSS exhibits a substantially reduced lattice thermal conductivity (<i>k</i><sub>l</sub>) of 0.82 W/mK, which is 2.5 times lower than that in LSSS (2.09 W/mK). The ultralow <i>k</i><sub>l</sub> of LPSS is strongly influenced by the presence of a valence band antibonding effect and Pb-dominated flat vibrational modes in the 0–2 THz frequency range, substantially enhancing three-phonon scattering channels, as evidenced by the distinct features in the weighted phase space. Additionally, the “double rattler” involving the LiS<sub>4</sub> and PbS<sub>8</sub> polyhedra in LPSS exhibits weak interactions, leading to significant anharmonicity and low <i>k</i><sub>l</sub>. The variation in the local crystal structures is manifested in the electronic band structures and phonon dispersion of these materials. These observations found in this study further enhance the considerable potential for investigating multielement systems and device applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12722–12732"},"PeriodicalIF":5.5,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007481","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tailoring LaCoO3 Perovskite Oxides via Ce Substitution and Nanofiber Architecture for Enhanced Electrochemical Storage Performance 通过Ce取代和纳米纤维结构定制LaCoO3钙钛矿氧化物以增强电化学存储性能
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-26 DOI: 10.1021/acsaem.5c01271
Jingrui Cao, Liyuan Liu, Bin Han, Zhiqiang Wang, Bin Li*, Muslum Demir and Pianpian Ma*, 
{"title":"Tailoring LaCoO3 Perovskite Oxides via Ce Substitution and Nanofiber Architecture for Enhanced Electrochemical Storage Performance","authors":"Jingrui Cao,&nbsp;Liyuan Liu,&nbsp;Bin Han,&nbsp;Zhiqiang Wang,&nbsp;Bin Li*,&nbsp;Muslum Demir and Pianpian Ma*,&nbsp;","doi":"10.1021/acsaem.5c01271","DOIUrl":"https://doi.org/10.1021/acsaem.5c01271","url":null,"abstract":"<p >Perovskite oxides offer great potential for supercapacitors thanks to their redox activity and structural tunability. However, their practical application is hindered by issues such as phase stability and low conductivity. Herein, La<sub>1–<i>x</i></sub>Ce<sub><i>x</i></sub>CoO<sub>3−δ</sub> (<i>x</i> = 0, 0.05, 0.1, 0.15, and 0.2) perovskite nanofibers were synthesized via the electrospinning–calcination method. As Ce substitution increased, the perovskite transitioned from a single hexagonal phase to a dual-phase (hexagonal and cubic) structure. Given that the as-constructed cubic phase and nanofiber morphology are more thermodynamically stable than the hexagonal phase in Co-based perovskites, Ce substitution was found to enhance the overall structural stability. Moreover, Ce substitution affected the oxygen vacancy concentration, with the highest concentration observed at <i>x</i> = 0.1, resulting in an optimal value of 267.9 F g<sup>–1</sup> at a current density of 1 A g<sup>–1</sup>. This was attributed to its relatively intact nanofiber structure providing abundant active sites and the lowest internal resistance. A supercapacitor device using La<sub>0.9</sub>Ce<sub>0.1</sub>CoO<sub>3</sub>@Ni-foam serving as the positive electrode and activated carbon (AC)@Ni-foam as the negative electrode achieved an energy density of 11.4 W h·kg<sup>–1</sup> at a power density of 775.1 W·kg<sup>–1</sup>. After 5000 charge–discharge cycles at 1 A g<sup>–1</sup>, the device retained 90.42% of its initial capacitance. These results demonstrate that Ce substitution significantly improves the electrochemical and cycling performance of LaCoO<sub>3</sub>, offering a viable strategy for designing stable and high-performance supercapacitor electrodes.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12543–12552"},"PeriodicalIF":5.5,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fully Printed Thermogalvanic Modules for Low-Grade Energy Harvesting 用于低等级能量收集的全印刷热电模块
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-25 DOI: 10.1021/acsaem.5c02080
Pedro Candiotto de Oliveira, Naveed ul Hassan Alvi, Najmeh Zahabi, Filippa Wentz, Kathrin Freitag, Lars Herlogsson, Ujwala Ail, Zia Ullah Khan, Igor Zozoulenko, Reverant Crispin* and Dan Zhao*, 
{"title":"Fully Printed Thermogalvanic Modules for Low-Grade Energy Harvesting","authors":"Pedro Candiotto de Oliveira,&nbsp;Naveed ul Hassan Alvi,&nbsp;Najmeh Zahabi,&nbsp;Filippa Wentz,&nbsp;Kathrin Freitag,&nbsp;Lars Herlogsson,&nbsp;Ujwala Ail,&nbsp;Zia Ullah Khan,&nbsp;Igor Zozoulenko,&nbsp;Reverant Crispin* and Dan Zhao*,&nbsp;","doi":"10.1021/acsaem.5c02080","DOIUrl":"https://doi.org/10.1021/acsaem.5c02080","url":null,"abstract":"<p >Thermogalvanic cells offer a promising route for harvesting low-grade heat by utilizing temperature-dependent redox reactions at spatially separated electrodes. Their potential for low-cost, flexible, and sustainable energy conversion makes them attractive for scalable applications; however, practical implementation is limited by challenges in modular integration and manufacturability. Here, we report the development of a fully printed thermogalvanic module (TGM) that integrates screen-printed hybrid current collectors, activated carbon-based electrodes, an adhesive sealing layer, and a laser-drilled spacer. This fully additive and scalable fabrication strategy enables the precise assembly of complex architectures without traditional stacking or wiring. The resulting 36-cell TGM, employing widely available aqueous electrolytes, demonstrates a reproducible thermopower of 38 mV K<sup>–1</sup> and a peak output power of 9 μW under a modest 14 K temperature difference. This work demonstrates a practical pathway toward large-area printed thermogalvanic systems for ambient heat harvesting and paves the way for future integration into flexible and wearable energy platforms.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12868–12877"},"PeriodicalIF":5.5,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsaem.5c02080","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Lattice-Matched CdS@Ag2S Core–Shell Structures on g-C3N4: A High-Performance Photocatalyst for Hydrogen Evolution and Pollutant Degradation under Visible Light 晶格匹配CdS@Ag2S g-C3N4的核壳结构:一种高性能可见光下的氢演化和污染物降解光催化剂
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-25 DOI: 10.1021/acsaem.5c02363
Santu Shrestha, Ga Hyeon Ha, Narayan Gyawali, Subas Acharya, Insup Lee, Harshvardhan Mohan, Taeho Shin and Jae Ryang Hahn*, 
{"title":"Lattice-Matched CdS@Ag2S Core–Shell Structures on g-C3N4: A High-Performance Photocatalyst for Hydrogen Evolution and Pollutant Degradation under Visible Light","authors":"Santu Shrestha,&nbsp;Ga Hyeon Ha,&nbsp;Narayan Gyawali,&nbsp;Subas Acharya,&nbsp;Insup Lee,&nbsp;Harshvardhan Mohan,&nbsp;Taeho Shin and Jae Ryang Hahn*,&nbsp;","doi":"10.1021/acsaem.5c02363","DOIUrl":"https://doi.org/10.1021/acsaem.5c02363","url":null,"abstract":"<p >A CdS@Ag<sub>2</sub>S core–shell architecture (CSAS) was fabricated via a low-temperature cation-exchange reaction between CdS and AgNO<sub>3</sub>, followed by hydrothermal integration with graphitic carbon nitride to form a CdS@Ag<sub>2</sub>S–g-C<sub>3</sub>N<sub>4</sub> (CSAS–g) composite. The development of a lattice-matched built-in electric field at the CSAS effectively overcame key limitations of conventional heterojunctions such as random material combinations, lattice mismatches, and high interfacial resistance, thereby significantly enhancing photocatalytic efficiency. The CSAS–g composite demonstrated remarkable bifunctional performance, achieving a significant H<sub>2</sub> production rate (1497.2 μmol g<sup>–1</sup> h<sup>–1</sup>), corresponding to a solar-to-hydrogen efficiency (1.63%) and an apparent quantum efficiency of 3.62%─which are 35.4 and 2.1 times higher than those of CdS nanoparticles (CdS-NPs) and CSAS, respectively. Additionally, CSAS–g exhibited outstanding photocatalytic decomposition of several pollutants, including bisphenol A, methylene blue, Rhodamine 6G, and Congo red. Notably, the methylene blue degradation rate of CSAS–g was 937.5% higher than that of photolysis and significantly outperformed CdS-NPs, CSAS, and g-C<sub>3</sub>N<sub>4</sub>. The exceptional photocatalytic efficacy and durability of CSAS–g were ascribed to the cooperative effects of the core–shell structure and g-C<sub>3</sub>N<sub>4</sub> integration, which resulted in superior light absorption, efficient charge separation, accelerated interfacial charge transport, and an abundance of active centers. Furthermore, the core–shell design provided enhanced photocorrosion resistance, ensuring long-term stability. This study highlights the transformative potential of lattice-matched core–shell heterostructures in advancing next-generation photocatalysts for renewable hydrogen production and pollution control.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12969–12983"},"PeriodicalIF":5.5,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Probing Expired Metformin as a Host to Modulate Active Sites for Carbon-Neutral Hydrogen Production: A Multi-Analytical Approach to Trigger Total Water Splitting Activity 探测过期二甲双胍作为调节碳中性氢生产活性位点的宿主:触发总水分解活性的多分析方法
IF 5.5 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-08-25 DOI: 10.1021/acsaem.5c01900
Thanikachalam Akshy, Thanikachalam Ajith, Dhanasingh Thiruvengadam, Mayakrishnan Raj kumar and Jayaraman Jayabharathi*, 
{"title":"Probing Expired Metformin as a Host to Modulate Active Sites for Carbon-Neutral Hydrogen Production: A Multi-Analytical Approach to Trigger Total Water Splitting Activity","authors":"Thanikachalam Akshy,&nbsp;Thanikachalam Ajith,&nbsp;Dhanasingh Thiruvengadam,&nbsp;Mayakrishnan Raj kumar and Jayaraman Jayabharathi*,&nbsp;","doi":"10.1021/acsaem.5c01900","DOIUrl":"https://doi.org/10.1021/acsaem.5c01900","url":null,"abstract":"<p >A nickel-based electrocatalyst for carbon-neutral hydrogen production could be developed via a meticulous synthetic strategy of tuning nickel oxidation states using the same scaffold host. We used expired metformin (MET) as a host for strategic tuning of Ni oxidation states in Ni-derived electrocatalysts (Ni-MET), namely, Ni<sup>2+</sup>-doped metformin (Ni2MET) and Ni<sup>0</sup>-doped metformin (Ni0MET), which improved the catalytic activity due to synergistic Ni–N interactions. The Ni2MET and Ni0MET catalyzed the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) with overpotentials of 361 mV (61 mV dec<sup>–1</sup>; 2.6 Ω) and 276 mV (71 mV dec<sup>–1</sup>; 3.1 Ω) to attain 50 mA cm<sup>–2</sup>, respectively. The optimized Ni2MET and Ni0MET exhibit higher TOFs (0.4073 and 0.3254 s<sup>–1</sup>, respectively) with faradaic efficiencies of 98.03 and 91%, respectively. The long-term stability of Ni2MET and Ni0MET over 100 h supported their robustness. The kinetic study via operando EIS reveals less resistance with more conductivity and enhanced kinetics of Ni2MET and Ni0MET. The improved activity was sustained by the Bode study at various potentials. The low activation energy of Ni2MET (2.21 and 2.86 kJ mol<sup>–1</sup>) signifies its potential for the OER and HER. The higher rate constant derived from Trumpet plot revealing that Ni2MET at various pH inferring rapid formation of gas bubbles. Finally, the alkaline and solar-driven electrolyzer Ni2MET//Ni0MET shows a low cell voltage of 1.48 V to attain 10 mA cm<sup>–2</sup> with great catalytic stability (100 h). All of the results explored that the metformin scaffold host ensured even dispersion and stabilization of Ni-active sites in a corrosive environment. The scaffold’s substantial stability is attributed to the N-rich core with extensive H-bonding and van der Waals forces, promoting electron rearrangement to lower the energy barrier, which unlocks the potential of metformin-based electrocatalysts in future energy applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12780–12799"},"PeriodicalIF":5.5,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007370","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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