Pub Date : 2024-07-17DOI: 10.1016/j.joule.2024.06.021
The identification of green strategies for ammonia production is critical, and nitrate reduction has emerged as a promising approach. In a recent issue of Nature Catalysis, Tayyebi et al. reported unprecedented ammonia production rates via bias-free photochemical nitrate reduction coupled with glycerol oxidation.
{"title":"Toward photovalorization of waste at scale?","authors":"","doi":"10.1016/j.joule.2024.06.021","DOIUrl":"10.1016/j.joule.2024.06.021","url":null,"abstract":"<div><p>The identification of green strategies for ammonia production is critical, and nitrate reduction has emerged as a promising approach. In a recent issue of <em>Nature Catalysis</em>, Tayyebi et al. reported unprecedented ammonia production rates via bias-free photochemical nitrate reduction coupled with glycerol oxidation.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":38.6,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141631766","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 : 2024-07-15DOI: 10.1016/j.joule.2024.06.015
Integrating metal-halide perovskites with the industrially textured Czochralski silicon for perovskite/silicon tandem cells shows great promise for low-cost manufacturing and ideal light trapping. However, the conformal growth of high-quality perovskite film on fully textured silicon remains challenging due to the lack of effective regulation of structural evolution and residual strains. Here, we report a strain regulation strategy by forming a 3D/3D perovskite heterojunction at the buried interface through a vacuum-deposition method applicable to pyramidal texture. By tailoring the composition of buried buffer 3D perovskite, a controllable compressive strain is applied to the upper photoactive 3D perovskite, alleviating its residual tensile stress. We demonstrate that this strained heterostructure promotes the preferred crystal growth, reduces interfacial defect-induced recombination, and facilitates charge extraction. As a result, the fully textured perovskite/silicon tandem cell achieves a certified steady-state efficiency of 31.5% and retains over 95% of its initial efficiency after 800 h of continuous operation.
{"title":"Strained heterojunction enables high-performance, fully textured perovskite/silicon tandem solar cells","authors":"","doi":"10.1016/j.joule.2024.06.015","DOIUrl":"https://doi.org/10.1016/j.joule.2024.06.015","url":null,"abstract":"<p>Integrating metal-halide perovskites with the industrially textured Czochralski silicon for perovskite/silicon tandem cells shows great promise for low-cost manufacturing and ideal light trapping. However, the conformal growth of high-quality perovskite film on fully textured silicon remains challenging due to the lack of effective regulation of structural evolution and residual strains. Here, we report a strain regulation strategy by forming a 3D/3D perovskite heterojunction at the buried interface through a vacuum-deposition method applicable to pyramidal texture. By tailoring the composition of buried buffer 3D perovskite, a controllable compressive strain is applied to the upper photoactive 3D perovskite, alleviating its residual tensile stress. We demonstrate that this strained heterostructure promotes the preferred crystal growth, reduces interfacial defect-induced recombination, and facilitates charge extraction. As a result, the fully textured perovskite/silicon tandem cell achieves a certified steady-state efficiency of 31.5% and retains over 95% of its initial efficiency after 800 h of continuous operation.</p>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141618425","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 : 2024-06-19DOI: 10.1016/j.joule.2024.03.017
Jia-Ning Liu , Chang-Xin Zhao , Juan Wang , Xuan-Qi Fang , Chen-Xi Bi , Bo-Quan Li , Qiang Zhang
Refreshing the record of the electrocatalytic activity for bifunctional oxygen electrocatalysis is the first priority of developing next-generation rechargeable zinc-air batteries. A ΔE indicator to evaluate the bifunctional electrocatalytic activity has stagnated with a record of ΔE > 0.60 V for decades. Herein, a bifunctional oxygen electrocatalyst is developed to afford an ultrahigh bifunctional electrocatalytic activity of ΔE = 0.57 V and realize high-performance rechargeable zinc-air batteries. Specifically, atomically dispersed Fe-N-C sites and NiFeCe layered double hydroxides are integrated to afford a composite FeNC@LDH electrocatalyst, following the guidance of the data-driven analysis. The FeNC@LDH electrocatalyst demonstrates a record-breaking electrocatalytic activity of ΔE = 0.57 V, far exceeding the state-of-the-art level by ca. 60 mV. Practical ampere-hour-scale zinc-air batteries are constructed with a capacity of 6.4 Ah and cycle under 1.0 A and 1.0 Ah conditions. This work affords a record-breaking bifunctional electrocatalyst for ampere-hour-scale zinc-air batteries in future application scenarios.
{"title":"A data-driven bifunctional oxygen electrocatalyst with a record-breaking ΔE = 0.57 V for ampere-hour-scale zinc-air batteries","authors":"Jia-Ning Liu , Chang-Xin Zhao , Juan Wang , Xuan-Qi Fang , Chen-Xi Bi , Bo-Quan Li , Qiang Zhang","doi":"10.1016/j.joule.2024.03.017","DOIUrl":"10.1016/j.joule.2024.03.017","url":null,"abstract":"<div><p>Refreshing the record of the electrocatalytic activity for bifunctional oxygen electrocatalysis is the first priority of developing next-generation rechargeable zinc-air batteries. A Δ<em>E</em> indicator to evaluate the bifunctional electrocatalytic activity has stagnated with a record of Δ<em>E</em> > 0.60 V for decades. Herein, a bifunctional oxygen electrocatalyst is developed to afford an ultrahigh bifunctional electrocatalytic activity of Δ<em>E</em> = 0.57 V and realize high-performance rechargeable zinc-air batteries. Specifically, atomically dispersed Fe-N-C sites and NiFeCe layered double hydroxides are integrated to afford a composite FeNC@LDH electrocatalyst, following the guidance of the data-driven analysis. The FeNC@LDH electrocatalyst demonstrates a record-breaking electrocatalytic activity of Δ<em>E</em> = 0.57 V, far exceeding the state-of-the-art level by ca. 60 mV. Practical ampere-hour-scale zinc-air batteries are constructed with a capacity of 6.4 Ah and cycle under 1.0 A and 1.0 Ah conditions. This work affords a record-breaking bifunctional electrocatalyst for ampere-hour-scale zinc-air batteries in future application scenarios.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140622983","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 : 2024-06-19DOI: 10.1016/j.joule.2024.05.010
Eddie Sun , Amitava Sarkar , Marco Gigantino , Richard Randall , Shaffiq Jaffer , Jimmy Rojas , Shang Zhai , Arun Majumdar
Amitava Sarkar is a corporate research scientist for North America at TotalEnergies and a resident visiting scientist at Stanford University working to develop disruptive, no/low-carbon sustainable technologies to decarbonize the chemical industry. He is active in TotalEnergies’ open innovation effort through research and development collaborations and strategic partnerships with various research institutions around the world.
Shaffiq Jaffer is the vice president of corporate science and technology projects in North America at TotalEnergies. He is engaged across the research ecosystem with relationships and investments in academia, startups, and private research companies for the purpose of bringing value to TotalEnergies and its partners.
Arun Majumdar is the inaugural dean of the Stanford Doerr School of Sustainability, the Jay Precourt provostial chair professor at Stanford University, a faculty in the Department of Mechanical Engineering, and a senior fellow and former director of the Stanford Precourt Institute for Energy. He served in the Obama administration as the founding director of the US Department of Energy’s Advanced Research Projects Agency-Energy (ARPA-E) (2009–2012), the acting undersecretary for energy (2011–2012), and as the vice chair of the secretary of energy advisory board (2014–2017). Dr. Majumdar is a member of the US National Academy of Sciences, US National Academy of Engineering, and the American Academy of Arts and Sciences.
Eddie Sun, Marco Gigantino, Richard Randall, Jimmy Rojas, and Shang Zhai were PhD students/postdoctoral scholars at Stanford University at the time of writing. Jimmy Rojas is now the founder and chief executive officer at EvolOH, and Shang Zhai is now an assistant professor in the Department of Mechanical and Aerospace Engineering (with a joint appointment in the School of Earth Sciences) at Ohio State University.
{"title":"Requirements for CO2-free hydrogen production at scale","authors":"Eddie Sun , Amitava Sarkar , Marco Gigantino , Richard Randall , Shaffiq Jaffer , Jimmy Rojas , Shang Zhai , Arun Majumdar","doi":"10.1016/j.joule.2024.05.010","DOIUrl":"10.1016/j.joule.2024.05.010","url":null,"abstract":"<div><p>Amitava Sarkar is a corporate research scientist for North America at TotalEnergies and a resident visiting scientist at Stanford University working to develop disruptive, no/low-carbon sustainable technologies to decarbonize the chemical industry. He is active in TotalEnergies’ open innovation effort through research and development collaborations and strategic partnerships with various research institutions around the world.</p><p>Shaffiq Jaffer is the vice president of corporate science and technology projects in North America at TotalEnergies. He is engaged across the research ecosystem with relationships and investments in academia, startups, and private research companies for the purpose of bringing value to TotalEnergies and its partners.</p><p>Arun Majumdar is the inaugural dean of the Stanford Doerr School of Sustainability, the Jay Precourt provostial chair professor at Stanford University, a faculty in the Department of Mechanical Engineering, and a senior fellow and former director of the Stanford Precourt Institute for Energy. He served in the Obama administration as the founding director of the US Department of Energy’s Advanced Research Projects Agency-Energy (ARPA-E) (2009–2012), the acting undersecretary for energy (2011–2012), and as the vice chair of the secretary of energy advisory board (2014–2017). Dr. Majumdar is a member of the US National Academy of Sciences, US National Academy of Engineering, and the American Academy of Arts and Sciences.</p><p>Eddie Sun, Marco Gigantino, Richard Randall, Jimmy Rojas, and Shang Zhai were PhD students/postdoctoral scholars at Stanford University at the time of writing. Jimmy Rojas is now the founder and chief executive officer at EvolOH, and Shang Zhai is now an assistant professor in the Department of Mechanical and Aerospace Engineering (with a joint appointment in the School of Earth Sciences) at Ohio State University.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141304646","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 : 2024-06-19DOI: 10.1016/j.joule.2024.05.009
Subir Majumder , Lin Dong , Fatemeh Doudi , Yuting Cai , Chao Tian , Dileep Kalathil , Kevin Ding , Anupam A. Thatte , Na Li , Le Xie
Large language models (LLMs) as ChatBots have drawn remarkable attention thanks to their versatile capability in natural language processing as well as in a wide range of tasks. While there has been great enthusiasm toward adopting such foundational model-based artificial intelligence tools in all sectors possible, the capabilities and limitations of such LLMs in improving the operation of the electric energy sector need to be explored, and this commentary identifies fruitful directions in this regard. Key future research directions include data collection systems for fine-tuning LLMs, embedding power system-specific tools in the LLMs, and retrieval augmented generation (RAG)-based knowledge pool to improve the quality of LLM responses and LLMs in safety-critical use cases.
{"title":"Exploring the capabilities and limitations of large language models in the electric energy sector","authors":"Subir Majumder , Lin Dong , Fatemeh Doudi , Yuting Cai , Chao Tian , Dileep Kalathil , Kevin Ding , Anupam A. Thatte , Na Li , Le Xie","doi":"10.1016/j.joule.2024.05.009","DOIUrl":"10.1016/j.joule.2024.05.009","url":null,"abstract":"<div><p>Large language models (LLMs) as ChatBots have drawn remarkable attention thanks to their versatile capability in natural language processing as well as in a wide range of tasks. While there has been great enthusiasm toward adopting such foundational model-based artificial intelligence tools in all sectors possible, the capabilities and limitations of such LLMs in improving the operation of the electric energy sector need to be explored, and this commentary identifies fruitful directions in this regard. Key future research directions include data collection systems for fine-tuning LLMs, embedding power system-specific tools in the LLMs, and retrieval augmented generation (RAG)-based knowledge pool to improve the quality of LLM responses and LLMs in safety-critical use cases.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425248","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 : 2024-06-19DOI: 10.1016/j.joule.2024.04.003
An L. Phan , Phung M.L. Le , Chunsheng Wang
Sulfurized polyacrylonitrile (SPAN) is emerging as a promising cathode for high-energy Li metal batteries. The transition-metal-free nature, high capacity, good sustainability, and low cost serve as competitive advantages of SPAN over conventional layered-oxide counterparts. The unique structure of SPAN with abundant covalent C–S and N–S bonds enables it to achieve high electrochemical performance even in lean electrolyte conditions. Despite great research progress, the current performance of Li/SPAN batteries still falls far behind its true potential. Here, we thoroughly analyze the energy density and cycle life of practical Li/SPAN cells based on our in-house-developed models. Besides, using Sand’s equation, we derive the requirements for Li/SPAN cells to achieve a reasonable power density and discuss their implications. Our analyses address critical issues of Li/SPAN on both material and cell levels, with an emphasis on particularly crucial details that are often overlooked or misunderstood. Accordingly, the challenges and directions for future Li/SPAN research are indicated.
{"title":"Realizing high-energy and long-life Li/SPAN batteries","authors":"An L. Phan , Phung M.L. Le , Chunsheng Wang","doi":"10.1016/j.joule.2024.04.003","DOIUrl":"10.1016/j.joule.2024.04.003","url":null,"abstract":"<div><p>Sulfurized polyacrylonitrile (SPAN) is emerging as a promising cathode for high-energy Li metal batteries. The transition-metal-free nature, high capacity, good sustainability, and low cost serve as competitive advantages of SPAN over conventional layered-oxide counterparts. The unique structure of SPAN with abundant covalent C–S and N–S bonds enables it to achieve high electrochemical performance even in lean electrolyte conditions. Despite great research progress, the current performance of Li/SPAN batteries still falls far behind its true potential. Here, we thoroughly analyze the energy density and cycle life of practical Li/SPAN cells based on our in-house-developed models. Besides, using Sand’s equation, we derive the requirements for Li/SPAN cells to achieve a reasonable power density and discuss their implications. Our analyses address critical issues of Li/SPAN on both material and cell levels, with an emphasis on particularly crucial details that are often overlooked or misunderstood. Accordingly, the challenges and directions for future Li/SPAN research are indicated.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140846064","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 : 2024-06-19DOI: 10.1016/j.joule.2024.04.012
Qiqi Tang , Binbin Jiang , Keli Wang , Wu Wang , Baohai Jia , Tianpeng Ding , Zhenlong Huang , Yuan Lin , Jiaqing He
More than 60% of the energy in the world is wasted during the energy conversion processes but can be potentially collected by thermoelectric (TE) technology. Recently, entropy engineering has been applied in the TE community, yielding numerous high-entropy material systems that exhibit outstanding TE performance. This review outlines the design principles for entropy-stabilized TE materials. Subsequently, it discusses the impact of high entropy on electrical and thermal transport properties. Furthermore, the research advancements of various high-entropy TE material systems are summarized, encompassing IV–VI compounds, half-Heusler (HH) compounds, liquid-like materials, oxide-based ceramics, and other relevant systems. Finally, the conclusion and outlook for high-entropy TE materials are elucidated. Only small regions of high-entropy TE materials have been investigated so far, and there will be vast space that remains to be explored. High-entropy TE materials will be one of the core strategies in the TE community if the optimization mechanism is completely understood.
世界上超过 60% 的能量在能量转换过程中被浪费掉了,但热电(TE)技术却有可能将其收集起来。最近,熵工程已被应用于热电技术领域,产生了许多表现出卓越热电技术性能的高熵材料系统。本综述概述了熵稳定 TE 材料的设计原则。随后,它讨论了高熵对电气和热传输特性的影响。此外,还总结了各种高熵 TE 材料系统的研究进展,包括 IV-VI 化合物、半休斯勒 (HH) 化合物、类液态材料、氧化物基陶瓷和其他相关系统。最后,阐明了高熵 TE 材料的结论和前景。迄今为止,人们只研究了高熵 TE 材料的一小部分,还有广阔的空间有待探索。如果能完全理解优化机制,高熵 TE 材料将成为 TE 界的核心战略之一。
{"title":"High-entropy thermoelectric materials","authors":"Qiqi Tang , Binbin Jiang , Keli Wang , Wu Wang , Baohai Jia , Tianpeng Ding , Zhenlong Huang , Yuan Lin , Jiaqing He","doi":"10.1016/j.joule.2024.04.012","DOIUrl":"10.1016/j.joule.2024.04.012","url":null,"abstract":"<div><p>More than 60% of the energy in the world is wasted during the energy conversion processes but can be potentially collected by thermoelectric (TE) technology. Recently, entropy engineering has been applied in the TE community, yielding numerous high-entropy material systems that exhibit outstanding TE performance. This review outlines the design principles for entropy-stabilized TE materials. Subsequently, it discusses the impact of high entropy on electrical and thermal transport properties. Furthermore, the research advancements of various high-entropy TE material systems are summarized, encompassing IV–VI compounds, half-Heusler (HH) compounds, liquid-like materials, oxide-based ceramics, and other relevant systems. Finally, the conclusion and outlook for high-entropy TE materials are elucidated. Only small regions of high-entropy TE materials have been investigated so far, and there will be vast space that remains to be explored. High-entropy TE materials will be one of the core strategies in the TE community if the optimization mechanism is completely understood.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140920035","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 : 2024-06-19DOI: 10.1016/j.joule.2024.02.027
Bjørt Óladóttir Joensen , José A. Zamora Zeledón , Lena Trotochaud , Andrea Sartori , Marta Mirolo , Asger Barkholt Moss , Sahil Garg , Ib Chorkendorff , Jakub Drnec , Brian Seger , Qiucheng Xu
In zero-gap CO2 electrolyzers, maintaining the balance of water and cations is crucial. Excessive accumulation at the cathode causes performance degradation, leading to flooding and salt precipitation. Using operando wide-angle X-ray scattering and X-ray fluorescence techniques, we observed the dynamic evolution of H2O and Cs+ inside a membrane electrode assembly. Our findings indicate that Cs+ movement across the membrane from the anode to the cathode is governed by migration and drags H2O via electroosmosis. H2O diffusion then allows Cs+ diffusion further within the gas diffusion electrode. When decreasing the applied voltage, the concentration gradient causes Cs+ to quickly diffuse back to the anode. The H2O content in the macro-porous layer remains at the same level, thus showcasing an origin of gas diffusion electrode (GDE) flooding. By regulating the electrolyte concentration, we deconvolute the correlation of water and cations for selectivity changes. Our work underscores the significance of water/cation management strategies in zero-gap electrolyzers.
在零间隙一氧化碳电解槽中,保持水和阳离子的平衡至关重要。阴极的过度积累会导致性能下降,造成水浸和盐沉淀。我们利用广角 X 射线散射和 X 射线荧光技术,观察了膜电极组件内 HO 和 Cs 的动态演变。我们的研究结果表明,Cs 在膜上从阳极向阴极的移动受迁移的支配,并通过电渗作用拖动 HO。然后,HO 扩散允许 Cs 在气体扩散电极内进一步扩散。当降低外加电压时,浓度梯度会使 Cs 迅速扩散回阳极。大孔层中的 HO 含量保持不变,从而显示了气体扩散电极(GDE)泛滥的起源。通过调节电解质浓度,我们解除了水和阳离子对选择性变化的相关性。我们的工作强调了零间隙电解槽中水/阳离子管理策略的重要性。
{"title":"Unveiling transport mechanisms of cesium and water in operando zero-gap CO2 electrolyzers","authors":"Bjørt Óladóttir Joensen , José A. Zamora Zeledón , Lena Trotochaud , Andrea Sartori , Marta Mirolo , Asger Barkholt Moss , Sahil Garg , Ib Chorkendorff , Jakub Drnec , Brian Seger , Qiucheng Xu","doi":"10.1016/j.joule.2024.02.027","DOIUrl":"10.1016/j.joule.2024.02.027","url":null,"abstract":"<div><p>In zero-gap CO<sub>2</sub> electrolyzers, maintaining the balance of water and cations is crucial. Excessive accumulation at the cathode causes performance degradation, leading to flooding and salt precipitation. Using <em>operando</em> wide-angle X-ray scattering and X-ray fluorescence techniques, we observed the dynamic evolution of H<sub>2</sub>O and Cs<sup>+</sup> inside a membrane electrode assembly. Our findings indicate that Cs<sup>+</sup> movement across the membrane from the anode to the cathode is governed by migration and drags H<sub>2</sub>O via electroosmosis. H<sub>2</sub>O diffusion then allows Cs<sup>+</sup> diffusion further within the gas diffusion electrode. When decreasing the applied voltage, the concentration gradient causes Cs<sup>+</sup> to quickly diffuse back to the anode. The H<sub>2</sub>O content in the macro-porous layer remains at the same level, thus showcasing an origin of gas diffusion electrode (GDE) flooding. By regulating the electrolyte concentration, we deconvolute the correlation of water and cations for selectivity changes. Our work underscores the significance of water/cation management strategies in zero-gap electrolyzers.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140173451","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 : 2024-06-19DOI: 10.1016/j.joule.2024.03.005
Zian Xu , Jian Zhu , Zheng Shu , Yu Xia , Rouxi Chen , Shaoqing Chen , Yu Wang , Lin Zeng , Jiacheng Wang , Yongqing Cai , Shi Chen , Fuqiang Huang , Hsing-Lin Wang
Metal aggregation, caused by high current density or long-cycling catalysis, severely affects the stability of ruthenium (Ru)-based catalysts toward hydrogen evolution reaction (HER). Herein, we constructed an anti-growth strategy of phosphorus (P)-induced Ru clusters (1.3 nm) integrated with adjacent Ru single atoms on nitrogen (N)-doped carbon fibers (RuSA/NP-PNCFs) for ultra-stable HER. The RuSA/NP-PNCFs exhibit outstanding activity (8 and 132 mV at 10 and 1,000 mA cm−2) and record durability (100,000 cycles and 1,000 h at 600 mA cm−2). Thanks to the optimized binding energy and orbital interaction between Ru and P/N, the size variation is only 0.8 nm, and single atoms are also well preserved. Both experiments and theoretical simulations indicate that the heteroatom P can not only boost the capacity of H2O dissociation but also suppress the aggregation of Ru clusters and single atoms during HER. This work provides an effective strategy for designing stable metal cluster-single-atom systems for advanced electrocatalysts.
高电流密度或长周期催化导致的金属聚集严重影响了基于钌(Ru)的催化剂在氢进化反应(HER)中的稳定性。在此,我们构建了一种磷(P)诱导的 Ru 簇(1.3 nm)与掺杂氮(N)的碳纤维上的相邻 Ru 单原子集成的抗生长策略(RuSA/NP-PNCFs),用于超稳定 HER。RuSA/NP-PNCFs 具有出色的活性(10 mA cm-2 和 1,000 mA cm-2 时分别为 8 mV 和 132 mV)和创纪录的耐久性(600 mA cm-2 时分别为 100,000 次循环和 1,000 小时)。由于 Ru 和 P/N 之间的结合能和轨道相互作用得到了优化,其尺寸变化仅为 0.8 纳米,而且单原子也得到了很好的保留。实验和理论模拟都表明,杂原子 P 不仅能提高 H2O 的解离能力,还能抑制 HER 过程中 Ru 簇和单个原子的聚集。这项工作为设计用于先进电催化剂的稳定金属团簇-单原子体系提供了有效的策略。
{"title":"Phosphorus-induced anti-growth of ruthenium clusters-single atoms for ultra-stable hydrogen evolution over 100,000 cycles","authors":"Zian Xu , Jian Zhu , Zheng Shu , Yu Xia , Rouxi Chen , Shaoqing Chen , Yu Wang , Lin Zeng , Jiacheng Wang , Yongqing Cai , Shi Chen , Fuqiang Huang , Hsing-Lin Wang","doi":"10.1016/j.joule.2024.03.005","DOIUrl":"10.1016/j.joule.2024.03.005","url":null,"abstract":"<div><p>Metal aggregation, caused by high current density or long-cycling catalysis, severely affects the stability of ruthenium (Ru)-based catalysts toward hydrogen evolution reaction (HER). Herein, we constructed an anti-growth strategy of phosphorus (P)-induced Ru clusters (1.3 nm) integrated with adjacent Ru single atoms on nitrogen (N)-doped carbon fibers (Ru<sub>SA/NP</sub>-PNCFs) for ultra-stable HER. The Ru<sub>SA/NP</sub>-PNCFs exhibit outstanding activity (8 and 132 mV at 10 and 1,000 mA cm<sup>−2</sup>) and record durability (100,000 cycles and 1,000 h at 600 mA cm<sup>−2</sup>). Thanks to the optimized binding energy and orbital interaction between Ru and P/N, the size variation is only 0.8 nm, and single atoms are also well preserved. Both experiments and theoretical simulations indicate that the heteroatom P can not only boost the capacity of H<sub>2</sub>O dissociation but also suppress the aggregation of Ru clusters and single atoms during HER. This work provides an effective strategy for designing stable metal cluster-single-atom systems for advanced electrocatalysts.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140624836","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 : 2024-06-19DOI: 10.1016/j.joule.2024.02.020
Nanlin Guo , Sihui Chen , Jun Tao , Yang Liu , Jiayu Wan , Xin Li
Accurate prediction of battery lifetime is critical for ensuring timely maintenance and safety of batteries. Although data-driven methods have made significant progress, their model accuracy is often hampered by a scarcity of labeled data. To address this challenge, we developed a semi-supervised learning technique named partial Bayesian co-training (PBCT), enhancing the modeling of battery lifetime prediction. Leveraging the low-cost unlabeled data, our model extracts hidden information to improve the understanding of the underlying data patterns and achieve higher lifetime prediction accuracy. PBCT outperforms existing approaches by up to 21.9% on lifetime prediction accuracy, with negligible overhead for data acquisition. Moreover, our research suggests that incorporating unlabeled data into the training process can help to uncover critical factors that impact battery lifetime, which may be overlooked with a limited number of labeled data alone. The proposed semi-supervised approach sheds light on the future direction for efficient and explainable data-driven battery status estimation.
{"title":"Semi-supervised learning for explainable few-shot battery lifetime prediction","authors":"Nanlin Guo , Sihui Chen , Jun Tao , Yang Liu , Jiayu Wan , Xin Li","doi":"10.1016/j.joule.2024.02.020","DOIUrl":"10.1016/j.joule.2024.02.020","url":null,"abstract":"<div><p>Accurate prediction of battery lifetime is critical for ensuring timely maintenance and safety of batteries. Although data-driven methods have made significant progress, their model accuracy is often hampered by a scarcity of labeled data. To address this challenge, we developed a semi-supervised learning technique named partial Bayesian co-training (PBCT), enhancing the modeling of battery lifetime prediction. Leveraging the low-cost unlabeled data, our model extracts hidden information to improve the understanding of the underlying data patterns and achieve higher lifetime prediction accuracy. PBCT outperforms existing approaches by up to 21.9% on lifetime prediction accuracy, with negligible overhead for data acquisition. Moreover, our research suggests that incorporating unlabeled data into the training process can help to uncover critical factors that impact battery lifetime, which may be overlooked with a limited number of labeled data alone. The proposed semi-supervised approach sheds light on the future direction for efficient and explainable data-driven battery status estimation.</p></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":null,"pages":null},"PeriodicalIF":39.8,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140270171","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}