Pub Date : 2024-09-18DOI: 10.1038/s41560-024-01629-0
Betar M. Gallant
Improving lithium anode cycling has long relied on links between electrolyte bulk properties and the interphase formed on lithium, with little understanding of the transformation process. A study reveals factors governing structural changes around lithium ions at the onset of metal plating, illuminating an unseen step in the trajectory from ion to lithium metal.
{"title":"Mapping the uncharted interface","authors":"Betar M. Gallant","doi":"10.1038/s41560-024-01629-0","DOIUrl":"https://doi.org/10.1038/s41560-024-01629-0","url":null,"abstract":"Improving lithium anode cycling has long relied on links between electrolyte bulk properties and the interphase formed on lithium, with little understanding of the transformation process. A study reveals factors governing structural changes around lithium ions at the onset of metal plating, illuminating an unseen step in the trajectory from ion to lithium metal.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236822","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 : 2024-09-18DOI: 10.1038/s41560-024-01634-3
Sebastian Puls, Elina Nazmutdinova, Fariza Kalyk, Henry M. Woolley, Jesper Frost Thomsen, Zhu Cheng, Adrien Fauchier-Magnan, Ajay Gautam, Michael Gockeln, So-Yeon Ham, Md Toukir Hasan, Min-Gi Jeong, Daiki Hiraoka, Jong Seok Kim, Tobias Kutsch, Barthélémy Lelotte, Philip Minnmann, Vanessa Miß, Kota Motohashi, Douglas Lars Nelson, Frans Ooms, Francesco Piccolo, Christian Plank, Maria Rosner, Stephanie E. Sandoval, Eva Schlautmann, Robin Schuster, Dominic Spencer-Jolly, Yipeng Sun, Bairav S. Vishnugopi, Ruizhuo Zhang, Huang Zheng, Philipp Adelhelm, Torsten Brezesinski, Peter G. Bruce, Michael Danzer, Mario El Kazzi, Hubert Gasteiger, Kelsey B. Hatzell, Akitoshi Hayashi, Felix Hippauf, Jürgen Janek, Yoon Seok Jung, Matthew T. McDowell, Ying Shirley Meng, Partha P. Mukherjee, Saneyuki Ohno, Bernhard Roling, Atsushi Sakuda, Julian Schwenzel, Xueliang Sun, Claire Villevieille, Marnix Wagemaker, Wolfgang G. Zeier, Nella M. Vargas-Barbosa
The interlaboratory comparability and reproducibility of all-solid-state battery cell cycling performance are poorly understood due to the lack of standardized set-ups and assembly parameters. This study quantifies the extent of this variability by providing commercially sourced battery materials—LiNi0.6Mn0.2Co0.2O2 for the positive electrode, Li6PS5Cl as the solid electrolyte and indium for the negative electrode—to 21 research groups. Each group was asked to use their own cell assembly protocol but follow a specific electrochemical protocol. The results show large variability in assembly and electrochemical performance, including differences in processing pressures, pressing durations and In-to-Li ratios. Despite this, an initial open circuit voltage of 2.5 and 2.7 V vs Li+/Li is a good predictor of successful cycling for cells using these electroactive materials. We suggest a set of parameters for reporting all-solid-state battery cycling results and advocate for reporting data in triplicate.
由于缺乏标准化的设置和组装参数,人们对全固态电池电池循环性能的实验室间可比性和可重复性知之甚少。本研究通过向 21 个研究小组提供市售电池材料--正极为 LiNi0.6Mn0.2Co0.2O2,固态电解质为 Li6PS5Cl,负极为铟,来量化这种可变性的程度。每个小组都被要求使用自己的电池组装方案,但要遵循特定的电化学方案。结果显示,组装和电化学性能存在很大差异,包括加工压力、加压持续时间和铟锂比的不同。尽管如此,初始开路电压为 2.5 和 2.7 V vs Li+/Li,仍能很好地预测使用这些电活性材料的电池能否成功循环。我们提出了一套报告全固态电池循环结果的参数,并主张报告一式三份的数据。
{"title":"Benchmarking the reproducibility of all-solid-state battery cell performance","authors":"Sebastian Puls, Elina Nazmutdinova, Fariza Kalyk, Henry M. Woolley, Jesper Frost Thomsen, Zhu Cheng, Adrien Fauchier-Magnan, Ajay Gautam, Michael Gockeln, So-Yeon Ham, Md Toukir Hasan, Min-Gi Jeong, Daiki Hiraoka, Jong Seok Kim, Tobias Kutsch, Barthélémy Lelotte, Philip Minnmann, Vanessa Miß, Kota Motohashi, Douglas Lars Nelson, Frans Ooms, Francesco Piccolo, Christian Plank, Maria Rosner, Stephanie E. Sandoval, Eva Schlautmann, Robin Schuster, Dominic Spencer-Jolly, Yipeng Sun, Bairav S. Vishnugopi, Ruizhuo Zhang, Huang Zheng, Philipp Adelhelm, Torsten Brezesinski, Peter G. Bruce, Michael Danzer, Mario El Kazzi, Hubert Gasteiger, Kelsey B. Hatzell, Akitoshi Hayashi, Felix Hippauf, Jürgen Janek, Yoon Seok Jung, Matthew T. McDowell, Ying Shirley Meng, Partha P. Mukherjee, Saneyuki Ohno, Bernhard Roling, Atsushi Sakuda, Julian Schwenzel, Xueliang Sun, Claire Villevieille, Marnix Wagemaker, Wolfgang G. Zeier, Nella M. Vargas-Barbosa","doi":"10.1038/s41560-024-01634-3","DOIUrl":"https://doi.org/10.1038/s41560-024-01634-3","url":null,"abstract":"<p>The interlaboratory comparability and reproducibility of all-solid-state battery cell cycling performance are poorly understood due to the lack of standardized set-ups and assembly parameters. This study quantifies the extent of this variability by providing commercially sourced battery materials—LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> for the positive electrode, Li<sub>6</sub>PS<sub>5</sub>Cl as the solid electrolyte and indium for the negative electrode—to 21 research groups. Each group was asked to use their own cell assembly protocol but follow a specific electrochemical protocol. The results show large variability in assembly and electrochemical performance, including differences in processing pressures, pressing durations and In-to-Li ratios. Despite this, an initial open circuit voltage of 2.5 and 2.7 V vs Li<sup>+</sup>/Li is a good predictor of successful cycling for cells using these electroactive materials. We suggest a set of parameters for reporting all-solid-state battery cycling results and advocate for reporting data in triplicate.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236847","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 : 2024-09-18DOI: 10.1038/s41560-024-01631-6
Matteo C. Romano
Adsorption-based CO2 capture is characterized by significant interdependencies between sorbent properties, CO2 sources and process design. Research now underlines that a holistic approach is essential for designing high-performing materials and processes from techno-economic-environmental perspectives.
{"title":"MOFs, holistically","authors":"Matteo C. Romano","doi":"10.1038/s41560-024-01631-6","DOIUrl":"https://doi.org/10.1038/s41560-024-01631-6","url":null,"abstract":"Adsorption-based CO2 capture is characterized by significant interdependencies between sorbent properties, CO2 sources and process design. Research now underlines that a holistic approach is essential for designing high-performing materials and processes from techno-economic-environmental perspectives.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236845","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 : 2024-09-17DOI: 10.1038/s41560-024-01630-7
Elizabeth Doris
Clean energy presents opportunities to reduce poverty and improve air quality on federally recognized indigenous land in the continental United States. Analysis now provides a step change in our understanding of the potential benefits of renewable power development on reservation lands, increasing our understanding towards equitable energy transition.
{"title":"Refining Native American clean-energy opportunities","authors":"Elizabeth Doris","doi":"10.1038/s41560-024-01630-7","DOIUrl":"https://doi.org/10.1038/s41560-024-01630-7","url":null,"abstract":"Clean energy presents opportunities to reduce poverty and improve air quality on federally recognized indigenous land in the continental United States. Analysis now provides a step change in our understanding of the potential benefits of renewable power development on reservation lands, increasing our understanding towards equitable energy transition.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142235203","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 : 2024-09-16DOI: 10.1038/s41560-024-01620-9
Jan Figgener, Jonas van Ouwerkerk, David Haberschusz, Jakob Bors, Philipp Woerner, Marc Mennekes, Felix Hildenbrand, Christopher Hecht, Kai-Philipp Kairies, Oliver Wessels, Dirk Uwe Sauer
Home storage systems play an important role in the integration of residential photovoltaic systems and have recently experienced strong market growth worldwide. However, standardized methods for quantifying capacity fade during field operation are lacking, and therefore the European batteries regulation demands the development of reliable and transparent state of health estimations. Here we present real-world data from 21 privately operated lithium-ion systems in Germany, based on up to 8 years of high-resolution field measurements. We develop a scalable capacity estimation method based on the operational data and validate it through regular field capacity tests. The results show that systems lose about two to three percentage points of usable capacity per year on average. Our contribution includes the publication of an impactful dataset comprising approximately 106 system years, 14 billion data points and 146 gigabytes, aiming to address the shortage of public datasets in this field.
{"title":"Multi-year field measurements of home storage systems and their use in capacity estimation","authors":"Jan Figgener, Jonas van Ouwerkerk, David Haberschusz, Jakob Bors, Philipp Woerner, Marc Mennekes, Felix Hildenbrand, Christopher Hecht, Kai-Philipp Kairies, Oliver Wessels, Dirk Uwe Sauer","doi":"10.1038/s41560-024-01620-9","DOIUrl":"https://doi.org/10.1038/s41560-024-01620-9","url":null,"abstract":"<p>Home storage systems play an important role in the integration of residential photovoltaic systems and have recently experienced strong market growth worldwide. However, standardized methods for quantifying capacity fade during field operation are lacking, and therefore the European batteries regulation demands the development of reliable and transparent state of health estimations. Here we present real-world data from 21 privately operated lithium-ion systems in Germany, based on up to 8 years of high-resolution field measurements. We develop a scalable capacity estimation method based on the operational data and validate it through regular field capacity tests. The results show that systems lose about two to three percentage points of usable capacity per year on average. Our contribution includes the publication of an impactful dataset comprising approximately 106 system years, 14 billion data points and 146 gigabytes, aiming to address the shortage of public datasets in this field.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234490","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 : 2024-09-16DOI: 10.1038/s41560-024-01609-4
Stephanie Hirmer, Julia Tomei, Pu Yang, Alycia Leonard, Philipp Trotter, Ariane Millot, Florian Egli, Koen van Dam, Agnese Beltramo, Martin Stringer
Electricity access statistics used to track progress against the Sustainable Development Goal 7.1 set by the United Nations have significant uncertainties, which may bring into question the electrification status of at least 87.2 million people in sub-Saharan Africa. Consequently, we call for a re-evaluation of the definitions of electricity access used by international organizations and the methodologies applied to calculate them.
{"title":"Inconsistent measurement calls into question progress on electrification in sub-Saharan Africa","authors":"Stephanie Hirmer, Julia Tomei, Pu Yang, Alycia Leonard, Philipp Trotter, Ariane Millot, Florian Egli, Koen van Dam, Agnese Beltramo, Martin Stringer","doi":"10.1038/s41560-024-01609-4","DOIUrl":"https://doi.org/10.1038/s41560-024-01609-4","url":null,"abstract":"Electricity access statistics used to track progress against the Sustainable Development Goal 7.1 set by the United Nations have significant uncertainties, which may bring into question the electrification status of at least 87.2 million people in sub-Saharan Africa. Consequently, we call for a re-evaluation of the definitions of electricity access used by international organizations and the methodologies applied to calculate them.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234489","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}
Interfacial molecules have been demonstrated to improve the photovoltaic performance of perovskite solar cells (PSCs). However, the effect is influenced by the targeted substrate and, in particular, by its bond with the interfacial molecule. A weaker bonding of the interfacial molecule with the substrate usually implies a stronger bonding with the perovskite that could lead to uncontrollable insertion of the interfacial molecule into the perovskite bulk, resulting in device degradation. Here we select bis(2-aminoethyl) ether (BAE) as the interfacial molecule between the perovskite and the electron transport layer (ETL) in n–i–p PSCs and develop a strategy to harmonize the strength of the bilateral bonds of BAE. In particular, we manipulate the electronic structure of the ETL with doping to increase the strength of the BAE–ETL bond. This thereby results in a weakening of the BAE–perovskite bond. The harmonization in bilateral bonds of the interfacial molecule leads to PSCs with an efficiency surpassing 26.5% (certified as 26.31%) and improved stability.
{"title":"Harmonizing the bilateral bond strength of the interfacial molecule in perovskite solar cells","authors":"Qiuyang Li, Hong Liu, Cheng-Hung Hou, Haoming Yan, Shunde Li, Peng Chen, Hongyu Xu, Wen-Yi Yu, Yiping Zhao, Yanping Sui, Qixuan Zhong, Yongqiang Ji, Jing-Jong Shyue, Shuang Jia, Bo Yang, Pengyi Tang, Qihuang Gong, Lichen Zhao, Rui Zhu","doi":"10.1038/s41560-024-01642-3","DOIUrl":"https://doi.org/10.1038/s41560-024-01642-3","url":null,"abstract":"<p>Interfacial molecules have been demonstrated to improve the photovoltaic performance of perovskite solar cells (PSCs). However, the effect is influenced by the targeted substrate and, in particular, by its bond with the interfacial molecule. A weaker bonding of the interfacial molecule with the substrate usually implies a stronger bonding with the perovskite that could lead to uncontrollable insertion of the interfacial molecule into the perovskite bulk, resulting in device degradation. Here we select bis(2-aminoethyl) ether (BAE) as the interfacial molecule between the perovskite and the electron transport layer (ETL) in n–i–p PSCs and develop a strategy to harmonize the strength of the bilateral bonds of BAE. In particular, we manipulate the electronic structure of the ETL with doping to increase the strength of the BAE–ETL bond. This thereby results in a weakening of the BAE–perovskite bond. The harmonization in bilateral bonds of the interfacial molecule leads to PSCs with an efficiency surpassing 26.5% (certified as 26.31%) and improved stability.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234492","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}
Electrochemical reduction of CO2 (CO2RR) to multi-carbon products is a promising technology to store intermittent renewable electricity into high-added-value chemicals and close the carbon cycle. Its industrial scalability requires electrocatalysts to be highly selective to certain products, such as ethylene or ethanol. However, a substantial knowledge gap prevents the design of tailor-made materials, as the properties ruling the catalyst selectivity remain elusive. Here we combined in situ surface-enhanced Raman spectroscopy and density functional theory on Cu electrocatalysts to unveil the reaction scheme for CO2RR to C2+ products. Ethylene generation occurs when *OC–CO(H) dimers form via CO coupling on undercoordinated Cu sites. The ethanol route opens up only in the presence of highly compressed and distorted Cu domains with deep s-band states via the crucial intermediate *OCHCH2. By identifying and tracking the critical intermediates and specific active sites, our work provides guidelines to selectively decouple ethylene and ethanol production on rationally designed catalysts.
将二氧化碳(CO2RR)电化学还原为多碳产品,是将间歇性可再生能源电力储存为高附加值化学品并封闭碳循环的一项前景广阔的技术。其工业可扩展性要求电催化剂对某些产品(如乙烯或乙醇)具有高度选择性。然而,由于决定催化剂选择性的特性仍然难以捉摸,因此在设计定制材料方面存在巨大的知识差距。在此,我们结合铜电催化剂的原位表面增强拉曼光谱和密度泛函理论,揭示了 CO2RR 到 C2+ 产物的反应方案。当*OC-CO(H)二聚体在配位不足的 Cu 位点上通过 CO 偶联形成时,乙烯就生成了。乙醇路线只有在具有深 s 带状态的高度压缩和畸变 Cu 域存在的情况下,才会通过关键的中间体 *OCHCH2 出现。通过识别和跟踪关键的中间产物和特定的活性位点,我们的工作为在合理设计的催化剂上有选择地脱钩乙烯和乙醇的生产提供了指导。
{"title":"Key intermediates and Cu active sites for CO2 electroreduction to ethylene and ethanol","authors":"Chao Zhan, Federico Dattila, Clara Rettenmaier, Antonia Herzog, Matias Herran, Timon Wagner, Fabian Scholten, Arno Bergmann, Núria López, Beatriz Roldan Cuenya","doi":"10.1038/s41560-024-01633-4","DOIUrl":"https://doi.org/10.1038/s41560-024-01633-4","url":null,"abstract":"<p>Electrochemical reduction of CO<sub>2</sub> (CO<sub>2</sub>RR) to multi-carbon products is a promising technology to store intermittent renewable electricity into high-added-value chemicals and close the carbon cycle. Its industrial scalability requires electrocatalysts to be highly selective to certain products, such as ethylene or ethanol. However, a substantial knowledge gap prevents the design of tailor-made materials, as the properties ruling the catalyst selectivity remain elusive. Here we combined in situ surface-enhanced Raman spectroscopy and density functional theory on Cu electrocatalysts to unveil the reaction scheme for CO<sub>2</sub>RR to C<sub>2+</sub> products. Ethylene generation occurs when *OC–CO(H) dimers form via CO coupling on undercoordinated Cu sites. The ethanol route opens up only in the presence of highly compressed and distorted Cu domains with deep <i>s</i>-band states via the crucial intermediate *OCHCH<sub>2</sub>. By identifying and tracking the critical intermediates and specific active sites, our work provides guidelines to selectively decouple ethylene and ethanol production on rationally designed catalysts.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142166500","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 : 2024-09-03DOI: 10.1038/s41560-024-01628-1
Timo Boehler, Dominic Bresser
Nickel-rich lithium-ion cathode materials face severe structural and interfacial instabilities when cycled at high potentials and high degrees of delithiation. Now, a LiNi0.8Mn0.1Co0.1O2 material with a complementary composition and structure gradient, composed of an ordered, layered Co-poor bulk phase and a Co-enriched disordered rock-salt surface layer, is shown to efficiently address the issues.
{"title":"Preserving order by controlled disorder","authors":"Timo Boehler, Dominic Bresser","doi":"10.1038/s41560-024-01628-1","DOIUrl":"https://doi.org/10.1038/s41560-024-01628-1","url":null,"abstract":"Nickel-rich lithium-ion cathode materials face severe structural and interfacial instabilities when cycled at high potentials and high degrees of delithiation. Now, a LiNi0.8Mn0.1Co0.1O2 material with a complementary composition and structure gradient, composed of an ordered, layered Co-poor bulk phase and a Co-enriched disordered rock-salt surface layer, is shown to efficiently address the issues.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142123616","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 : 2024-08-26DOI: 10.1038/s41560-024-01583-x
Jin Suntivich, Geoffroy Hautier, Ismaila Dabo, Ethan J. Crumlin, Dhananjay Kumar, Tanja Cuk
The oxygen evolution reaction is crucial to sustainable electro- and photo-electrochemical approaches to chemical energy production (for example, H2). Although mechanistic descriptions of the oxygen evolution reaction have been proposed, the frontier challenge is to extract the molecular details of its elementary steps. Here we discuss how advances in spectroscopy and theory are allowing for configurations of reaction intermediates to be elucidated, distinguishing between experimental approaches (static and dynamic) across a range of surface oxygen binding energies on catalysts (from ruthenium to titanium oxides). We outline how interpreting X-ray and optical spectra relies on established and newly implemented computational techniques. A key emphasis is on detecting adsorbed oxygen intermediates at the oxide/water interface by their chemical composition, electronic and vibrational levels and ion–electron kinetic pathways. Integrating the computational advances with the experimental spectra along these lines could ultimately resolve the elementary steps, elucidating how each intermediate leads to another during oxygen evolution reaction.
氧进化反应对于以可持续的电化学和光电化学方法生产化学能(如 H2)至关重要。虽然已经提出了氧进化反应的机理描述,但前沿挑战是提取其基本步骤的分子细节。在此,我们将讨论光谱学和理论的进步如何使反应中间产物的构型得以阐明,并区分催化剂(从钌到钛氧化物)表面氧结合能范围内的实验方法(静态和动态)。我们概述了 X 射线和光学光谱的解释如何依赖于已有的和新实施的计算技术。重点是通过化学成分、电子和振动水平以及离子-电子动力学路径来检测氧化物/水界面上吸附的氧中间体。按照这些思路将计算进展与实验光谱相结合,最终可以解决基本步骤问题,阐明在氧进化反应过程中每个中间体如何导致另一个中间体。
{"title":"Probing intermediate configurations of oxygen evolution catalysis across the light spectrum","authors":"Jin Suntivich, Geoffroy Hautier, Ismaila Dabo, Ethan J. Crumlin, Dhananjay Kumar, Tanja Cuk","doi":"10.1038/s41560-024-01583-x","DOIUrl":"https://doi.org/10.1038/s41560-024-01583-x","url":null,"abstract":"<p>The oxygen evolution reaction is crucial to sustainable electro- and photo-electrochemical approaches to chemical energy production (for example, H<sub>2</sub>). Although mechanistic descriptions of the oxygen evolution reaction have been proposed, the frontier challenge is to extract the molecular details of its elementary steps. Here we discuss how advances in spectroscopy and theory are allowing for configurations of reaction intermediates to be elucidated, distinguishing between experimental approaches (static and dynamic) across a range of surface oxygen binding energies on catalysts (from ruthenium to titanium oxides). We outline how interpreting X-ray and optical spectra relies on established and newly implemented computational techniques. A key emphasis is on detecting adsorbed oxygen intermediates at the oxide/water interface by their chemical composition, electronic and vibrational levels and ion–electron kinetic pathways. Integrating the computational advances with the experimental spectra along these lines could ultimately resolve the elementary steps, elucidating how each intermediate leads to another during oxygen evolution reaction.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085368","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}