Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102172
Sanghyun Bae , Thomas Moehl , David Yong , Peng Zeng , S. David Tilley
The development of efficient, stable, and earth-abundant photoanodes for solar water oxidation is critical to advancing photoelectrochemical and photocatalytic systems for large-scale renewable fuel production. Here, we demonstrate that p-type Cu2O, typically studied as a photocathode material, can be used as a high-performance photoanode through judicious engineering of charge carrier-selective contacts on thermally oxidized Cu2O sheets. The introduction of Ga2O3, TiO2, and indium tin oxide (ITO) layers as an electron-selective back contact, combined with Al2O3, Au, and Ni front layers, significantly enhanced charge separation and electron transfer. The champion Cu2O photoanode exhibited a photocurrent density of 8.65 mA cm−2 at 1.23 V vs. the reversible hydrogen electrode in alkaline media, which is the highest reported for metal oxide photoanodes. These findings highlight the pivotal role of charge carrier-selective interface engineering in broadening the scope of available semiconductor materials for photo(electro)catalytic oxidation reactions, irrespective of the doping type of the light-absorbing material.
开发高效、稳定、资源丰富的太阳能水氧化光阳极对于推进大规模可再生燃料生产的光电化学和光催化系统至关重要。在这里,我们证明了通常作为光电阴极材料研究的p型Cu2O,可以通过在热氧化Cu2O片上明智地设计电荷载流子选择接触来用作高性能的光阳极。引入Ga2O3、TiO2和铟锡氧化物(ITO)层作为电子选择的后接触层,结合Al2O3、Au和Ni前缘层,显著增强了电荷分离和电子转移。与碱性介质中可逆氢电极相比,冠军Cu2O光阳极在1.23 V下的光电流密度为8.65 mA cm−2,是目前报道的金属氧化物光阳极中最高的。这些发现强调了电荷载流子选择界面工程在扩大光(电)催化氧化反应可用半导体材料的范围方面的关键作用,而不考虑光吸收材料的掺杂类型。
{"title":"A p-type Cu2O photoanode for solar water oxidation","authors":"Sanghyun Bae , Thomas Moehl , David Yong , Peng Zeng , S. David Tilley","doi":"10.1016/j.joule.2025.102172","DOIUrl":"10.1016/j.joule.2025.102172","url":null,"abstract":"<div><div>The development of efficient, stable, and earth-abundant photoanodes for solar water oxidation is critical to advancing photoelectrochemical and photocatalytic systems for large-scale renewable fuel production. Here, we demonstrate that p-type Cu<sub>2</sub>O, typically studied as a photocathode material, can be used as a high-performance photoanode through judicious engineering of charge carrier-selective contacts on thermally oxidized Cu<sub>2</sub>O sheets. The introduction of Ga<sub>2</sub>O<sub>3</sub>, TiO<sub>2</sub>, and indium tin oxide (ITO) layers as an electron-selective back contact, combined with Al<sub>2</sub>O<sub>3</sub>, Au, and Ni front layers, significantly enhanced charge separation and electron transfer. The champion Cu<sub>2</sub>O photoanode exhibited a photocurrent density of 8.65 mA cm<sup>−2</sup> at 1.23 V vs. the reversible hydrogen electrode in alkaline media, which is the highest reported for metal oxide photoanodes. These findings highlight the pivotal role of charge carrier-selective interface engineering in broadening the scope of available semiconductor materials for photo(electro)catalytic oxidation reactions, irrespective of the doping type of the light-absorbing material.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102172"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145382566","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102222
Shanshan Gao , Ah Hyun Shin , Seong Sik Shin
While perovskite solar cells (PSCs) continue to break records in efficiency, their commercialization has been hampered by limitations in long-term stability. In a recent issue of Nature Energy, Zhao et al. revealed a new degradation mechanism under realistic dynamic cycling and proposed an innovative solution to improve stability.
{"title":"Perovskite solar cells remain stable under realistic day-night cycling conditions","authors":"Shanshan Gao , Ah Hyun Shin , Seong Sik Shin","doi":"10.1016/j.joule.2025.102222","DOIUrl":"10.1016/j.joule.2025.102222","url":null,"abstract":"<div><div>While perovskite solar cells (PSCs) continue to break records in efficiency, their commercialization has been hampered by limitations in long-term stability. In a recent issue of <em>Nature Energy</em>, Zhao et al. revealed a new degradation mechanism under realistic dynamic cycling and proposed an innovative solution to improve stability.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102222"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145545817","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102211
Ruy Sebastian Bonilla
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Sebastian Bonilla is an associate professor of materials at the University of Oxford, recognized for his work on silicon-based solar energy. He completed his doctorate at Oxford in 2015 and has held prestigious fellowships from EPSRC and the Royal Academy of Engineering. In 2022, he received the Philip Leverhulme Prize for Engineering. His research focuses on functional thin-film materials for photovoltaics, with major contributions to interface engineering, silicon passivation, hydrogen incorporation, and device reliability. His work bridges fundamental science and industrial application, advancing the performance and durability of solar and optoelectronic devices.
{"title":"The impact of transparent conducting electrodes on tandem solar cell efficiency","authors":"Ruy Sebastian Bonilla","doi":"10.1016/j.joule.2025.102211","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102211","url":null,"abstract":"<span><figure><span><img alt=\"\" height=\"243\" src=\"https://ars.els-cdn.com/content/image/1-s2.0-S2542435125003927-fx1.jpg\"/><ol><li><span><span>Download: <span>Download high-res image (295KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span>Sebastian Bonilla is an associate professor of materials at the University of Oxford, recognized for his work on silicon-based solar energy. He completed his doctorate at Oxford in 2015 and has held prestigious fellowships from EPSRC and the Royal Academy of Engineering. In 2022, he received the Philip Leverhulme Prize for Engineering. His research focuses on functional thin-film materials for photovoltaics, with major contributions to interface engineering, silicon passivation, hydrogen incorporation, and device reliability. His work bridges fundamental science and industrial application, advancing the performance and durability of solar and optoelectronic devices.","PeriodicalId":343,"journal":{"name":"Joule","volume":"70 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145545747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102135
Xinkang Wang , Jifa Wu , Siyu Zhao , Mingqing Chen , Tianyuan Shi , Xianglun Xie , Qingqing Bai , Jialong Xie , Lianjie Zhang , Dongge Ma , Junwu Chen
The realization of highly efficient thick-film organic solar cells (OSCs) is a key path to reaching high-throughput organic photovoltaics. Herein, we demonstrate an additive strategy mediated by tribromopyrimidine (TBP) for optimizing of dielectric constant (εr) of organic semiconductor materials along with prolonged exciton diffusion length (LD) and enhanced vertical phase separation morphology. Based on 100-, 300-, and 500-nm-thick D18:L8-BO active layers, the TBP-treated binary OSCs showed power conversion efficiencies (PCEs) of 20.87%, 19.23%, and 17.82%, respectively, remarkably higher than those of 18.25%, 16.69%, and 13.52% of the corresponding control devices. A certified PCE of 19.23%, a record efficiency, and an exceptional high fill factor of 78.02% were achieved with the TBP-treated 300-nm-thick OSCs. Furthermore, enhanced device stabilities were demonstrated with the TBP-treated devices, retaining 87.9%, 79.4%, and 93.7% of the initial under continuous operational illumination (1,000 h), thermal aging (85°C, 720 h), and storage in air (720 h), respectively.
{"title":"Elevating dielectric constant via additive engineering: Achieving 19.23% certified efficiency in thick-film binary organic solar cells","authors":"Xinkang Wang , Jifa Wu , Siyu Zhao , Mingqing Chen , Tianyuan Shi , Xianglun Xie , Qingqing Bai , Jialong Xie , Lianjie Zhang , Dongge Ma , Junwu Chen","doi":"10.1016/j.joule.2025.102135","DOIUrl":"10.1016/j.joule.2025.102135","url":null,"abstract":"<div><div>The realization of highly efficient thick-film organic solar cells (OSCs) is a key path to reaching high-throughput organic photovoltaics. Herein, we demonstrate an additive strategy mediated by tribromopyrimidine (TBP) for optimizing of dielectric constant (ε<sub>r</sub>) of organic semiconductor materials along with prolonged exciton diffusion length (<em>L</em><sub>D</sub>) and enhanced vertical phase separation morphology. Based on 100-, 300-, and 500-nm-thick D18:L8-BO active layers, the TBP-treated binary OSCs showed power conversion efficiencies (PCEs) of 20.87%, 19.23%, and 17.82%, respectively, remarkably higher than those of 18.25%, 16.69%, and 13.52% of the corresponding control devices. A certified PCE of 19.23%, a record efficiency, and an exceptional high fill factor of 78.02% were achieved with the TBP-treated 300-nm-thick OSCs. Furthermore, enhanced device stabilities were demonstrated with the TBP-treated devices, retaining 87.9%, 79.4%, and 93.7% of the initial under continuous operational illumination (1,000 h), thermal aging (85°C, 720 h), and storage in air (720 h), respectively.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102135"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145103671","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102144
Francesco Lombardi , Koen van Greevenbroek , Aleksander Grochowicz , Michael Lau , Fabian Neumann , Neha Patankar , Oskar Vågerö
Cost-optimizing energy planning models are widespread in supporting energy transition planning decisions. Nonetheless, finding a “cost-optimal” planning strategy provides only a false sense of certainty. Stakeholders may prefer other economically comparable alternatives due to unaccounted-for features. Multi-objective or robust optimization, among others, can efficiently explore alternatives whose desired secondary features are well defined. “Modeling to generate alternatives” (MGA) explores alternatives systematically, including alternatives whose features, such as social viability, are hard to model, albeit key to practical implementation. Computational and interpretation barriers hindered past MGA usage and integration with other methods, but recent developments enable going beyond such barriers. We synthesize such developments and provide practical recommendations for applying MGA in five levels of increasing benefit. Even the simplest levels, requiring little computational effort, can substantially improve the quality of energy planning analyses. At the highest level of integration, MGA can facilitate identifying consensus strategies, accelerating the energy transition.
{"title":"Near-optimal energy planning strategies with modeling to generate alternatives to flexibly explore practically desirable options","authors":"Francesco Lombardi , Koen van Greevenbroek , Aleksander Grochowicz , Michael Lau , Fabian Neumann , Neha Patankar , Oskar Vågerö","doi":"10.1016/j.joule.2025.102144","DOIUrl":"10.1016/j.joule.2025.102144","url":null,"abstract":"<div><div>Cost-optimizing energy planning models are widespread in supporting energy transition planning decisions. Nonetheless, finding a “cost-optimal” planning strategy provides only a false sense of certainty. Stakeholders may prefer other economically comparable alternatives due to unaccounted-for features. Multi-objective or robust optimization, among others, can efficiently explore alternatives whose desired secondary features are well defined. “Modeling to generate alternatives” (MGA) explores alternatives systematically, including alternatives whose features, such as social viability, are hard to model, albeit key to practical implementation. Computational and interpretation barriers hindered past MGA usage and integration with other methods, but recent developments enable going beyond such barriers. We synthesize such developments and provide practical recommendations for applying MGA in five levels of increasing benefit. Even the simplest levels, requiring little computational effort, can substantially improve the quality of energy planning analyses. At the highest level of integration, MGA can facilitate identifying consensus strategies, accelerating the energy transition.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102144"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203903","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102176
Gun Jang , Sang Baek Kim , Wonji Jung , Hye Rin Park , Hao Fu , Sung Pil Hong , Min Jun Hwang , Hongdae Lee , Dong Wook Kim , Jee Yeon Kim , Changhoon Oh , Ho Seok Park , Hui-Ming Cheng
Here, we design an energy-efficient ion management and high-performance energy storage system based on a redox-active symmetric cell based on a divalent and halide dual-ion storage mechanism of V2O3 nanocrystal/carbon hybrids grown on reduced graphene oxide (V2O3@C/rGO). Experimental and computational analyses confirm the Ca2+ insertion-based ion storage and redox-mediating Br− conversion mechanism of the V2O3@C/rGO. The symmetric cells of two V2O3@C/rGO electrodes can function as an energy-dense aqueous divalent metal-halogen battery with a high rate and long cycles, as well as an energy-efficient redox-active capacitive deionization (RACDI) device with high salt adsorption capacity and rate in both high and low concentrations of wastewater. Particularly, the total energy consumption of our RACDI is 76 Wh kg−1, which is lower than that of existing CDI technologies, by means of spontaneous electrode regeneration without an ion-exchange membrane. This work provides a new concept of highly efficient and stable energy storage-desalination integrated functional systems for a sustainable wastewater-energy nexus.
{"title":"Divalent and halide dual-ion storage of a redox-active symmetric cell for an efficient wastewater-energy nexus","authors":"Gun Jang , Sang Baek Kim , Wonji Jung , Hye Rin Park , Hao Fu , Sung Pil Hong , Min Jun Hwang , Hongdae Lee , Dong Wook Kim , Jee Yeon Kim , Changhoon Oh , Ho Seok Park , Hui-Ming Cheng","doi":"10.1016/j.joule.2025.102176","DOIUrl":"10.1016/j.joule.2025.102176","url":null,"abstract":"<div><div>Here, we design an energy-efficient ion management and high-performance energy storage system based on a redox-active symmetric cell based on a divalent and halide dual-ion storage mechanism of V<sub>2</sub>O<sub>3</sub> nanocrystal/carbon hybrids grown on reduced graphene oxide (V<sub>2</sub>O<sub>3</sub>@C/rGO). Experimental and computational analyses confirm the Ca<sup>2+</sup> insertion-based ion storage and redox-mediating Br<sup>−</sup> conversion mechanism of the V<sub>2</sub>O<sub>3</sub>@C/rGO. The symmetric cells of two V<sub>2</sub>O<sub>3</sub>@C/rGO electrodes can function as an energy-dense aqueous divalent metal-halogen battery with a high rate and long cycles, as well as an energy-efficient redox-active capacitive deionization (RACDI) device with high salt adsorption capacity and rate in both high and low concentrations of wastewater. Particularly, the total energy consumption of our RACDI is 76 Wh kg<sup>−1</sup>, which is lower than that of existing CDI technologies, by means of spontaneous electrode regeneration without an ion-exchange membrane. This work provides a new concept of highly efficient and stable energy storage-desalination integrated functional systems for a sustainable wastewater-energy nexus.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102176"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145382180","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102142
Yawei Niu , Shuyi Lin , Xiaorui Dong , Minhuan Wang , Yuzhen Zhang , Sihan Ning , Zhe Li , Jingyang Wang , Jun Yin , Shangshang Chen , Pengchen Zhu , Jia Zhu
Connecting a wide-band-gap (WBG) perovskite solar cell with a crystalline silicon (c-Si) cell enables the device to surpass the Shockley-Queisser (S-Q) limit of a single-junction solar cell. However, strain in WBG perovskites reduces the ion migration barrier and defect formation energy, severely impacting the efficiency and stability of tandem devices. Herein, we utilize benzamidinium chloride (BMCl), a molecule containing a deprotonation-resistant amidinium group, which occupies the A-site vacancy and interacts strongly with the [PbI6]4− octahedra to stabilize the crystal lattice. This strategy synergistically facilitates uniform compressive strain formation within perovskite films, increasing the ion migration barrier and defect formation energy. The optimized WBG single-junction perovskite (with a 1.67 eV band gap) and 4-terminal (4T) perovskite/Si tandem devices achieved power conversion efficiencies (PCEs) of 23.5% (22.9% certified) and 33.4%, respectively. Remarkably, the 4T tandem device showed no PCE decay after 48 days of operation under outdoor conditions, demonstrating superior real-world stability.
{"title":"Homogenizing strain via reinforced lattice interaction enables efficient and stable 4T perovskite/silicon tandem solar cells","authors":"Yawei Niu , Shuyi Lin , Xiaorui Dong , Minhuan Wang , Yuzhen Zhang , Sihan Ning , Zhe Li , Jingyang Wang , Jun Yin , Shangshang Chen , Pengchen Zhu , Jia Zhu","doi":"10.1016/j.joule.2025.102142","DOIUrl":"10.1016/j.joule.2025.102142","url":null,"abstract":"<div><div>Connecting a wide-band-gap (WBG) perovskite solar cell with a crystalline silicon (c-Si) cell enables the device to surpass the Shockley-Queisser (S-Q) limit of a single-junction solar cell. However, strain in WBG perovskites reduces the ion migration barrier and defect formation energy, severely impacting the efficiency and stability of tandem devices. Herein, we utilize benzamidinium chloride (BMCl), a molecule containing a deprotonation-resistant amidinium group, which occupies the A-site vacancy and interacts strongly with the [PbI<sub>6</sub>]<sup>4−</sup> octahedra to stabilize the crystal lattice. This strategy synergistically facilitates uniform compressive strain formation within perovskite films, increasing the ion migration barrier and defect formation energy. The optimized WBG single-junction perovskite (with a 1.67 eV band gap) and 4-terminal (4T) perovskite/Si tandem devices achieved power conversion efficiencies (PCEs) of 23.5% (22.9% certified) and 33.4%, respectively. Remarkably, the 4T tandem device showed no PCE decay after 48 days of operation under outdoor conditions, demonstrating superior real-world stability.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102142"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145141104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102163
Yifan Feng , Zhenyu Xing , Daoping Ye , Jin Niu , Tian Ma , Bowen Liu , Yi Wang , Bo Yin , Chong Cheng , Shuang Li
Although molybdenum nitride (Mo2N) demonstrates exceptional hydrogenation potential, its intrinsic catalytic potential is severely compromised by the unavoidable surface oxidative molybdenum trioxide (MoO3) layer, which severely masks active Mo2N sites for hydrogen dissociation. Here, we report a carbon-supported Mo2N architecture (Mo2N-C) with partially exposed Mo2N sites that strategically balances surface protection and active site accessibility. This engineered Mo2N-C catalyst achieves a CO2 conversion rate of 20.3% at 500°C, with a CO2:H2 ratio of 1:1 and a weight hourly space velocity (WHSV) of 3 × 105 mL gcat−1 h−1, representing a 7-fold enhancement over conventional Mo2N. Remarkably, under a WHSV of 3 × 106 mL gcat−1 h−1, the Mo2N-C catalyst demonstrates unprecedented CO productivity (146.94 × 10−5 molCO gcat−1 s−1), outperforming all reported non-precious metal catalysts. This work establishes a new paradigm for designing oxidation-resistant and high-performance metal nitride catalysts through interface engineering, opening alternative avenues and generalizable approaches for sustainable CO2 conversion technologies.
尽管氮化钼(Mo2N)表现出优异的加氢电位,但其固有的催化电位受到不可避免的表面氧化三氧化钼(MoO3)层的严重损害,该层严重掩盖了氢解离的活性Mo2N位点。在这里,我们报告了一种碳支撑的Mo2N结构(Mo2N- c),其部分暴露的Mo2N位点战略性地平衡了表面保护和活性位点的可及性。该Mo2N-C催化剂在500℃下的CO2转化率为20.3%,CO2:H2比为1:1,重量小时空速(WHSV)为3 × 105 mL gcat−1 h−1,比传统Mo2N提高了7倍。值得注意的是,在3 × 106 mL gcat−1 h−1的WHSV下,Mo2N-C催化剂表现出前所未有的CO产率(146.94 × 10−5 molCO gcat−1 s−1),优于所有报道的非贵金属催化剂。本研究为通过界面工程设计抗氧化和高性能金属氮化物催化剂建立了一个新的范例,为可持续的二氧化碳转化技术开辟了替代途径和可推广的方法。
{"title":"Carbon-supported molybdenum nitride with optimized triple-phase interfaces for unprecedented efficiency in reverse water-gas shift reactions","authors":"Yifan Feng , Zhenyu Xing , Daoping Ye , Jin Niu , Tian Ma , Bowen Liu , Yi Wang , Bo Yin , Chong Cheng , Shuang Li","doi":"10.1016/j.joule.2025.102163","DOIUrl":"10.1016/j.joule.2025.102163","url":null,"abstract":"<div><div>Although molybdenum nitride (Mo<sub>2</sub>N) demonstrates exceptional hydrogenation potential, its intrinsic catalytic potential is severely compromised by the unavoidable surface oxidative molybdenum trioxide (MoO<sub>3</sub>) layer, which severely masks active Mo<sub>2</sub>N sites for hydrogen dissociation. Here, we report a carbon-supported Mo<sub>2</sub>N architecture (Mo<sub>2</sub>N-C) with partially exposed Mo<sub>2</sub>N sites that strategically balances surface protection and active site accessibility. This engineered Mo<sub>2</sub>N-C catalyst achieves a CO<sub>2</sub> conversion rate of 20.3% at 500°C, with a CO<sub>2</sub>:H<sub>2</sub> ratio of 1:1 and a weight hourly space velocity (WHSV) of 3 × 10<sup>5</sup> mL g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>, representing a 7-fold enhancement over conventional Mo<sub>2</sub>N. Remarkably, under a WHSV of 3 × 10<sup>6</sup> mL g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>, the Mo<sub>2</sub>N-C catalyst demonstrates unprecedented CO productivity (146.94 × 10<sup>−5</sup> mol<sub>CO</sub> g<sub>cat</sub><sup>−1</sup> s<sup>−1</sup>), outperforming all reported non-precious metal catalysts. This work establishes a new paradigm for designing oxidation-resistant and high-performance metal nitride catalysts through interface engineering, opening alternative avenues and generalizable approaches for sustainable CO<sub>2</sub> conversion technologies.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102163"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255421","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-19DOI: 10.1016/j.joule.2025.102175
Souhardh Kotakadi , Jack Aspinall , Matthew Burton , Yi Liang , Yuichi Aihara , Mauro Pasta
Solid-state batteries promise higher energy density than current lithium-ion technology. To achieve this and address challenges associated with metallic lithium, zero-excess lithium configurations are required. Metallic interlayers at the negative electrode-electrolyte interface present a route to control plating morphology and improve lithium cycling efficiency, but their underlying mechanism remains unclear. Here, we systematically investigate the lithiation dynamics of bismuth, indium, silver, and magnesium interlayers using operando scanning electron microscopy. Solid solution-forming interlayers promote uniform plating and maintain structural integrity, while intermetallic-forming interlayers undergo mechanical failure due to volumetric changes. Heterogeneous lithiation arises from lithium diffusivity differences between phases. Three-electrode impedance spectroscopy and coulometric titration time analysis reveal that interlayer deposition onto the solid electrolyte maximizes electrochemically active contact with the current collector, reducing effective current density but increasing solid electrolyte interphase growth. Overall, plating morphology, mechanical stability, and cycling efficiency are governed by alloy nucleation behavior and lithium diffusivity.
{"title":"Impact of metallic interlayers at the lithium-Li6PS5Cl solid electrolyte interface","authors":"Souhardh Kotakadi , Jack Aspinall , Matthew Burton , Yi Liang , Yuichi Aihara , Mauro Pasta","doi":"10.1016/j.joule.2025.102175","DOIUrl":"10.1016/j.joule.2025.102175","url":null,"abstract":"<div><div>Solid-state batteries promise higher energy density than current lithium-ion technology. To achieve this and address challenges associated with metallic lithium, zero-excess lithium configurations are required. Metallic interlayers at the negative electrode-electrolyte interface present a route to control plating morphology and improve lithium cycling efficiency, but their underlying mechanism remains unclear. Here, we systematically investigate the lithiation dynamics of bismuth, indium, silver, and magnesium interlayers using <em>operando scanning electron microscopy</em>. Solid solution-forming interlayers promote uniform plating and maintain structural integrity, while intermetallic-forming interlayers undergo mechanical failure due to volumetric changes. Heterogeneous lithiation arises from lithium diffusivity differences between phases. Three-electrode impedance spectroscopy and coulometric titration time analysis reveal that interlayer deposition onto the solid electrolyte maximizes electrochemically active contact with the current collector, reducing effective current density but increasing solid electrolyte interphase growth. Overall, plating morphology, mechanical stability, and cycling efficiency are governed by alloy nucleation behavior and lithium diffusivity.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 11","pages":"Article 102175"},"PeriodicalIF":35.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145382179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-17DOI: 10.1016/j.joule.2025.102212
Jin Wen, Yuxuan Liu, Yinke Wang, Guihao Wang, Ningchong Zheng, Wennan Ou, Jinyan Guo, Jiajia Hong, Yijia Guo, Wenchi Kong, Anh Dinh Bui, Haowen Luo, Hieu Nguyen, Yuefeng Nie, Ke Xiao, Ludong Li, Hairen Tan
The buried heterointerface between hole transport layers (HTLs) and perovskite films critically determines the efficiency and stability of scalable perovskite solar modules. While self-assembled monolayer (SAM)-based HTLs enable record efficiencies in spin-coated devices, scalable blade coating often induces micron-scale nanogaps at the SAM/perovskite interface, causing non-radiative recombination and mechanical degradation. Here, we introduce a buried integrating-passivation nanostructure (BIPN) atop SAM, where inorganic oxide nanoparticles are utilized as mechanical reinforcements and passivating molecules function as chemical stabilizers, anchoring onto spherical surfaces via hydrogen bonding. This design effectively alleviates interfacial stress and minimizes nanoscale gaps, simultaneously decreasing defects and strengthening the buried interface. As a result, blade-coated perovskite solar cells achieve a power conversion efficiency of 26.0% (certified at 25.7%), while minimodules (20.25 cm2 aperture) deliver 22.5% efficiency and show no degradation after 2,100 h under the International Summit on Organic Photovoltaic Stability (ISOS)-L-1 condition.
{"title":"Buried heterointerface reinforcement with passivation-integrated nanostructures for efficient and stable perovskite solar modules","authors":"Jin Wen, Yuxuan Liu, Yinke Wang, Guihao Wang, Ningchong Zheng, Wennan Ou, Jinyan Guo, Jiajia Hong, Yijia Guo, Wenchi Kong, Anh Dinh Bui, Haowen Luo, Hieu Nguyen, Yuefeng Nie, Ke Xiao, Ludong Li, Hairen Tan","doi":"10.1016/j.joule.2025.102212","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102212","url":null,"abstract":"The buried heterointerface between hole transport layers (HTLs) and perovskite films critically determines the efficiency and stability of scalable perovskite solar modules. While self-assembled monolayer (SAM)-based HTLs enable record efficiencies in spin-coated devices, scalable blade coating often induces micron-scale nanogaps at the SAM/perovskite interface, causing non-radiative recombination and mechanical degradation. Here, we introduce a buried integrating-passivation nanostructure (BIPN) atop SAM, where inorganic oxide nanoparticles are utilized as mechanical reinforcements and passivating molecules function as chemical stabilizers, anchoring onto spherical surfaces via hydrogen bonding. This design effectively alleviates interfacial stress and minimizes nanoscale gaps, simultaneously decreasing defects and strengthening the buried interface. As a result, blade-coated perovskite solar cells achieve a power conversion efficiency of 26.0% (certified at 25.7%), while minimodules (20.25 cm<sup>2</sup> aperture) deliver 22.5% efficiency and show no degradation after 2,100 h under the International Summit on Organic Photovoltaic Stability (ISOS)-L-1 condition.","PeriodicalId":343,"journal":{"name":"Joule","volume":"43 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145531813","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}