Pub Date : 2024-10-07DOI: 10.1038/s41560-024-01639-y
Jie Xiao, Nicole Adelstein, Yujing Bi, Wenjuan Bian, Jordi Cabana, Corie L. Cobb, Yi Cui, Shen J. Dillon, Marca M. Doeff, Saiful M. Islam, Kevin Leung, Mengya Li, Feng Lin, Jun Liu, Hongmei Luo, Amy C. Marschilok, Ying Shirley Meng, Yue Qi, Ritu Sahore, Kayla G. Sprenger, Robert C. Tenent, Michael F. Toney, Wei Tong, Liwen F. Wan, Chongmin Wang, Stephen E. Weitzner, Bingbin Wu, Yaobin Xu
The cathode–electrolyte interphase plays a pivotal role in determining the usable capacity and cycling stability of electrochemical cells, yet it is overshadowed by its counterpart, the solid–electrolyte interphase. This is primarily due to the prevalence of side reactions, particularly at low potentials on the negative electrode, especially in state-of-the-art Li-ion batteries where the charge cutoff voltage is limited. However, as the quest for high-energy battery technologies intensifies, there is a pressing need to advance the study of cathode–electrolyte interphase properties. Here, we present a comprehensive approach to analyse the cathode–electrolyte interphase in battery systems. We underscore the importance of employing model cathode materials and coin cell protocols to establish baseline performance. Additionally, we delve into the factors behind the inconsistent and occasionally controversial findings related to the cathode–electrolyte interphase. We also address the challenges and opportunities in characterizing and simulating the cathode–electrolyte interphase, offering potential solutions to enhance its relevance to real-world applications.
{"title":"Assessing cathode–electrolyte interphases in batteries","authors":"Jie Xiao, Nicole Adelstein, Yujing Bi, Wenjuan Bian, Jordi Cabana, Corie L. Cobb, Yi Cui, Shen J. Dillon, Marca M. Doeff, Saiful M. Islam, Kevin Leung, Mengya Li, Feng Lin, Jun Liu, Hongmei Luo, Amy C. Marschilok, Ying Shirley Meng, Yue Qi, Ritu Sahore, Kayla G. Sprenger, Robert C. Tenent, Michael F. Toney, Wei Tong, Liwen F. Wan, Chongmin Wang, Stephen E. Weitzner, Bingbin Wu, Yaobin Xu","doi":"10.1038/s41560-024-01639-y","DOIUrl":"https://doi.org/10.1038/s41560-024-01639-y","url":null,"abstract":"<p>The cathode–electrolyte interphase plays a pivotal role in determining the usable capacity and cycling stability of electrochemical cells, yet it is overshadowed by its counterpart, the solid–electrolyte interphase. This is primarily due to the prevalence of side reactions, particularly at low potentials on the negative electrode, especially in state-of-the-art Li-ion batteries where the charge cutoff voltage is limited. However, as the quest for high-energy battery technologies intensifies, there is a pressing need to advance the study of cathode–electrolyte interphase properties. Here, we present a comprehensive approach to analyse the cathode–electrolyte interphase in battery systems. We underscore the importance of employing model cathode materials and coin cell protocols to establish baseline performance. Additionally, we delve into the factors behind the inconsistent and occasionally controversial findings related to the cathode–electrolyte interphase. We also address the challenges and opportunities in characterizing and simulating the cathode–electrolyte interphase, offering potential solutions to enhance its relevance to real-world applications.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"30 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142383663","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-07DOI: 10.1038/s41560-024-01632-5
Jiafeng Lei, Yi-Chun Lu
Deposition–dissolution reactions are key to the function of rechargeable batteries, but the limited reversibility of plating/stripping shortens their lifespan. Now, a liquid crystal interphase is shown to control deposition in preferred orientations, enabling dual-electrode-free batteries with enhanced reversibility and increased energy density.
{"title":"Building interphases for electrode-free batteries","authors":"Jiafeng Lei, Yi-Chun Lu","doi":"10.1038/s41560-024-01632-5","DOIUrl":"https://doi.org/10.1038/s41560-024-01632-5","url":null,"abstract":"Deposition–dissolution reactions are key to the function of rechargeable batteries, but the limited reversibility of plating/stripping shortens their lifespan. Now, a liquid crystal interphase is shown to control deposition in preferred orientations, enabling dual-electrode-free batteries with enhanced reversibility and increased energy density.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"1 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142383657","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-02DOI: 10.1038/s41560-024-01649-w
Anthony L. Cheng, Erica R. H. Fuchs, Jeremy J. Michalek
We analyse US Inflation Reduction Act (IRA) incentives for electric vehicle battery technology and supply chain decisions. We find that the total value of available credits exceeds estimated battery production costs, but qualifying for all available credits is difficult. IRA cell and module credits alone bring estimated US battery production costs in line with China. In contrast, IRA material extraction and processing credits are modest. IRA’s end-user purchase credits are restricted to electric vehicles whose battery supply chains exclude foreign entities of concern, including China. This incentivizes diversification of the entire supply chain, but leasing avoids these restrictions. Lithium iron phosphate batteries have potential to more easily reduce supply chain vulnerabilities and qualify for incentives, but they have smaller total available incentives than nickel/cobalt-based batteries. Overall, the IRA primarily incentivizes downstream battery manufacturing diversification, whereas upstream supply implications depend on automaker responses to foreign entities of concern and leasing rules.
我们分析了美国《通货膨胀削减法案》(IRA)对电动汽车电池技术和供应链决策的激励作用。我们发现,可用信用额度的总价值超过了估计的电池生产成本,但要获得所有可用信用额度却很困难。仅 IRA 电池和模块抵免就能使美国电池生产成本与中国持平。相比之下,IRA 的材料提取和加工抵免额度并不高。IRA 的最终用户购买信用额度仅限于电池供应链不包括包括中国在内的外国相关实体的电动汽车。这激励了整个供应链的多样化,但租赁避免了这些限制。磷酸铁锂电池有可能更容易减少供应链漏洞,并符合激励条件,但与镍基/钴基电池相比,其可用激励总额较小。总体而言,《综合减排法》主要激励下游电池制造多样化,而上游供应的影响则取决于汽车制造商对外国相关实体和租赁规则的反应。
{"title":"US industrial policy may reduce electric vehicle battery supply chain vulnerabilities and influence technology choice","authors":"Anthony L. Cheng, Erica R. H. Fuchs, Jeremy J. Michalek","doi":"10.1038/s41560-024-01649-w","DOIUrl":"https://doi.org/10.1038/s41560-024-01649-w","url":null,"abstract":"<p>We analyse US Inflation Reduction Act (IRA) incentives for electric vehicle battery technology and supply chain decisions. We find that the total value of available credits exceeds estimated battery production costs, but qualifying for all available credits is difficult. IRA cell and module credits alone bring estimated US battery production costs in line with China. In contrast, IRA material extraction and processing credits are modest. IRA’s end-user purchase credits are restricted to electric vehicles whose battery supply chains exclude foreign entities of concern, including China. This incentivizes diversification of the entire supply chain, but leasing avoids these restrictions. Lithium iron phosphate batteries have potential to more easily reduce supply chain vulnerabilities and qualify for incentives, but they have smaller total available incentives than nickel/cobalt-based batteries. Overall, the IRA primarily incentivizes downstream battery manufacturing diversification, whereas upstream supply implications depend on automaker responses to foreign entities of concern and leasing rules.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"22 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142362748","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Publisher Correction: 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/s41560-024-01659-8","DOIUrl":"https://doi.org/10.1038/s41560-024-01659-8","url":null,"abstract":"<p>Correction to: <i>Nature Energy</i> https://doi.org/10.1038/s41560-024-01642-3, published online 16 September 2024.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"17 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329627","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1038/s41560-024-01637-0
Selma Brynolf, Maria Grahn
Not all parts of the transport sector are easy to directly electrify, therefore liquid energy carriers with lower environmental impacts than fossil fuels are needed to aid decarbonization. Research now reports that synthetic fuels with optimized alkane/alcohol content are promising drop-in alternatives.
{"title":"Flexibility with low environmental impact","authors":"Selma Brynolf, Maria Grahn","doi":"10.1038/s41560-024-01637-0","DOIUrl":"10.1038/s41560-024-01637-0","url":null,"abstract":"Not all parts of the transport sector are easy to directly electrify, therefore liquid energy carriers with lower environmental impacts than fossil fuels are needed to aid decarbonization. Research now reports that synthetic fuels with optimized alkane/alcohol content are promising drop-in alternatives.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"9 10","pages":"1179-1180"},"PeriodicalIF":49.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324969","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1038/s41560-024-01640-5
L. van der Most, K. van der Wiel, R. M. J. Benders, P. W. Gerbens-Leenes, R. Bintanja
As Europe’s renewable energy capacities expand, electricity systems face increased risks of energy droughts—periods of low production coinciding with high demand. We evaluate characteristics of electricity variability due to weather variations by calculating 1,600 years of daily production and demand. Focusing on five European countries—chosen for their energy mix including hydropower—we find that energy droughts result from processes that cause (temporally) compounding impacts in the energy and meteorological system. These can turn what might have been short-term droughts into prolonged high unmet energy demand. For instance, low reservoir inflows in spring quadruple the chance of prolonged energy droughts: reduced snowpack and rainfall lower hydro availability but also dry out subsoils, increasing the chance of heatwaves and therewith extending the energy problems into summer. We identify and quantify three compounding energy/climate conditions and the associated characteristics and risks of multi-year energy droughts, crucial for informing future energy system design.
{"title":"Temporally compounding energy droughts in European electricity systems with hydropower","authors":"L. van der Most, K. van der Wiel, R. M. J. Benders, P. W. Gerbens-Leenes, R. Bintanja","doi":"10.1038/s41560-024-01640-5","DOIUrl":"https://doi.org/10.1038/s41560-024-01640-5","url":null,"abstract":"<p>As Europe’s renewable energy capacities expand, electricity systems face increased risks of energy droughts—periods of low production coinciding with high demand. We evaluate characteristics of electricity variability due to weather variations by calculating 1,600 years of daily production and demand. Focusing on five European countries—chosen for their energy mix including hydropower—we find that energy droughts result from processes that cause (temporally) compounding impacts in the energy and meteorological system. These can turn what might have been short-term droughts into prolonged high unmet energy demand. For instance, low reservoir inflows in spring quadruple the chance of prolonged energy droughts: reduced snowpack and rainfall lower hydro availability but also dry out subsoils, increasing the chance of heatwaves and therewith extending the energy problems into summer. We identify and quantify three compounding energy/climate conditions and the associated characteristics and risks of multi-year energy droughts, crucial for informing future energy system design.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"89 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324981","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1038/s41560-024-01624-5
Meinan He, Louis G. Hector Jr, Fang Dai, Fan Xu, Suryanarayana Kolluri, Nathaniel Hardin, Mei Cai
Lithium-metal battery (LMB) research and development has been ongoing for six decades across academia, industry and national laboratories. Despite this extensive effort, commercial LMBs have yet to displace, or offer a ready alternative to, lithium-ion batteries in electric vehicles (EVs). Here we explore some of the most critical industry needs that will have to be resolved to advance practical LMB designs for implementation in EVs. We begin our exploration with a brief overview of LMBs, then consider the following needs: energy density, anode thickness and cathode loading, electrolyte formulation and gas generation, electrolyte injection amount, cathode oxygen release, cell pressure control, cell format, cell manufacturing quality checks and battery modelling. We conclude with generic cell design recommendations for future LMB EV applications. Despite extensive research, lithium-metal batteries have not yet replaced lithium-ion batteries in electric vehicles. The authors explore critical industry needs for advancing lithium-metal battery designs for electric vehicles and conclude with cell design recommendations.
{"title":"Industry needs for practical lithium-metal battery designs in electric vehicles","authors":"Meinan He, Louis G. Hector Jr, Fang Dai, Fan Xu, Suryanarayana Kolluri, Nathaniel Hardin, Mei Cai","doi":"10.1038/s41560-024-01624-5","DOIUrl":"10.1038/s41560-024-01624-5","url":null,"abstract":"Lithium-metal battery (LMB) research and development has been ongoing for six decades across academia, industry and national laboratories. Despite this extensive effort, commercial LMBs have yet to displace, or offer a ready alternative to, lithium-ion batteries in electric vehicles (EVs). Here we explore some of the most critical industry needs that will have to be resolved to advance practical LMB designs for implementation in EVs. We begin our exploration with a brief overview of LMBs, then consider the following needs: energy density, anode thickness and cathode loading, electrolyte formulation and gas generation, electrolyte injection amount, cathode oxygen release, cell pressure control, cell format, cell manufacturing quality checks and battery modelling. We conclude with generic cell design recommendations for future LMB EV applications. Despite extensive research, lithium-metal batteries have not yet replaced lithium-ion batteries in electric vehicles. The authors explore critical industry needs for advancing lithium-metal battery designs for electric vehicles and conclude with cell design recommendations.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"9 10","pages":"1199-1205"},"PeriodicalIF":49.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324972","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1038/s41560-024-01606-7
M. Calcaterra, L. Aleluia Reis, P. Fragkos, T. Briera, H. S. de Boer, F. Egli, J. Emmerling, G. Iyer, S. Mittal, F. H. J. Polzin, M. W. J. L. Sanders, T. S. Schmidt, A. Serebriakova, B. Steffen, D. J. van de Ven, D. P. van Vuuren, P. Waidelich, M. Tavoni
Climate stabilization requires the mobilization of substantial investments in low- and zero-carbon technologies, especially in emerging and developing economies. However, access to stable and affordable finance varies dramatically across countries. Models used to evaluate the energy transition do not differentiate regional financing costs and therefore cannot study risk-sharing mechanisms for renewable electricity generation. In this study, we incorporated the empirically estimated cost of capital differentiated by country and technology into an ensemble of five climate–energy–economy models. We quantified the additional financing cost of decarbonization borne by developing regions and explored policies of risk premium convergence across countries. We found that alleviating financial constraints benefits both climate and equity as a result of more renewable and affordable energy in the developing world. This highlights the importance of fair finance for energy availability, affordability and sustainability, as well as the need to include financial considerations in model-based assessments. Fair finance in the energy sector is modelled in five climate–energy–economy models. The results show that convergence costs of capital could improve energy availability, affordability and sustainability in developing countries, thereby increasing the international equity of the energy transition.
{"title":"Reducing the cost of capital to finance the energy transition in developing countries","authors":"M. Calcaterra, L. Aleluia Reis, P. Fragkos, T. Briera, H. S. de Boer, F. Egli, J. Emmerling, G. Iyer, S. Mittal, F. H. J. Polzin, M. W. J. L. Sanders, T. S. Schmidt, A. Serebriakova, B. Steffen, D. J. van de Ven, D. P. van Vuuren, P. Waidelich, M. Tavoni","doi":"10.1038/s41560-024-01606-7","DOIUrl":"10.1038/s41560-024-01606-7","url":null,"abstract":"Climate stabilization requires the mobilization of substantial investments in low- and zero-carbon technologies, especially in emerging and developing economies. However, access to stable and affordable finance varies dramatically across countries. Models used to evaluate the energy transition do not differentiate regional financing costs and therefore cannot study risk-sharing mechanisms for renewable electricity generation. In this study, we incorporated the empirically estimated cost of capital differentiated by country and technology into an ensemble of five climate–energy–economy models. We quantified the additional financing cost of decarbonization borne by developing regions and explored policies of risk premium convergence across countries. We found that alleviating financial constraints benefits both climate and equity as a result of more renewable and affordable energy in the developing world. This highlights the importance of fair finance for energy availability, affordability and sustainability, as well as the need to include financial considerations in model-based assessments. Fair finance in the energy sector is modelled in five climate–energy–economy models. The results show that convergence costs of capital could improve energy availability, affordability and sustainability in developing countries, thereby increasing the international equity of the energy transition.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"9 10","pages":"1241-1251"},"PeriodicalIF":49.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41560-024-01606-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1038/s41560-024-01641-4
We identified temporally compounding meteorological conditions that increase the risk of low renewable electricity production during periods of high demand in five European countries with hydropower.
我们发现,在五个拥有水电的欧洲国家,在高需求时期,时间复合气象条件增加了可再生能源发电量低的风险。
{"title":"Weather conditions linked to energy droughts in electricity systems with hydropower","authors":"","doi":"10.1038/s41560-024-01641-4","DOIUrl":"https://doi.org/10.1038/s41560-024-01641-4","url":null,"abstract":"We identified temporally compounding meteorological conditions that increase the risk of low renewable electricity production during periods of high demand in five European countries with hydropower.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"8 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142328649","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-24DOI: 10.1038/s41560-024-01645-0
Zhanyou Xu, Ruihu Lu, Zih-Yi Lin, Weixing Wu, Hsin-Jung Tsai, Qian Lu, Yuguang C. Li, Sung-Fu Hung, Chunshan Song, Jimmy C. Yu, Ziyun Wang, Ying Wang
The electrochemical CO2 reduction reaction towards value-added fuel and feedstocks often relies on metal-based catalysts. Organic molecular catalysts, which are more acutely tunable than metal catalysts, are still unable to catalyse CO2 to hydrocarbons under industrially relevant current densities for long-term operation, and the catalytic mechanism is still elusive. Here we report 3,5-diamino-1,2,4-triazole-based membrane electrode assemblies for CO2-to-CH4 conversion with Faradaic efficiency of (52 ± 4)% and turnover frequency of 23,060 h−1 at 250 mA cm−2. Our mechanistic studies suggest that the CO2 reduction at the 3,5-diamino-1,2,4-triazole electrode proceeds through the intermediary *CO2–*COOH–*C(OH)2–*COH to produce CH4 due to the spatially distributed active sites and the suitable energy level of the molecular orbitals. A pilot system operated under a total current of 10 A (current density = 123 mA cm−2) for 10 h is able to produce CH4 at a rate of 23.0 mmol h−1.
{"title":"Electroreduction of CO2 to methane with triazole molecular catalysts","authors":"Zhanyou Xu, Ruihu Lu, Zih-Yi Lin, Weixing Wu, Hsin-Jung Tsai, Qian Lu, Yuguang C. Li, Sung-Fu Hung, Chunshan Song, Jimmy C. Yu, Ziyun Wang, Ying Wang","doi":"10.1038/s41560-024-01645-0","DOIUrl":"https://doi.org/10.1038/s41560-024-01645-0","url":null,"abstract":"<p>The electrochemical CO<sub>2</sub> reduction reaction towards value-added fuel and feedstocks often relies on metal-based catalysts. Organic molecular catalysts, which are more acutely tunable than metal catalysts, are still unable to catalyse CO<sub>2</sub> to hydrocarbons under industrially relevant current densities for long-term operation, and the catalytic mechanism is still elusive. Here we report 3,5-diamino-1,2,4-triazole-based membrane electrode assemblies for CO<sub>2</sub>-to-CH<sub>4</sub> conversion with Faradaic efficiency of (52 ± 4)% and turnover frequency of 23,060 h<sup>−1</sup> at 250 mA cm<sup>−2</sup>. Our mechanistic studies suggest that the CO<sub>2</sub> reduction at the 3,5-diamino-1,2,4-triazole electrode proceeds through the intermediary *CO<sub>2</sub>–*COOH–*C(OH)<sub>2</sub>–*COH to produce CH<sub>4</sub> due to the spatially distributed active sites and the suitable energy level of the molecular orbitals. A pilot system operated under a total current of 10 A (current density = 123 mA cm<sup>−2</sup>) for 10 h is able to produce CH<sub>4</sub> at a rate of 23.0 mmol h<sup>−1</sup>.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"1 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142313986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}