JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.07.001
Laura L. Driscoll , Abbey Jarvis , Rosie Madge , Elizabeth H. Driscoll , Jaime-Marie Price , Rob Sommerville , Felipe Schnaider Tontini , Mounib Bahri , Milon Miah , B. Layla Mehdi , Emma Kendrick , Nigel D. Browning , Phoebe K. Allan , Paul A. Anderson , Peter R. Slater
{"title":"Phase-selective recovery and regeneration of end-of-life electric vehicle blended cathodes via selective leaching and direct recycling","authors":"Laura L. Driscoll , Abbey Jarvis , Rosie Madge , Elizabeth H. Driscoll , Jaime-Marie Price , Rob Sommerville , Felipe Schnaider Tontini , Mounib Bahri , Milon Miah , B. Layla Mehdi , Emma Kendrick , Nigel D. Browning , Phoebe K. Allan , Paul A. Anderson , Peter R. Slater","doi":"10.1016/j.joule.2024.07.001","DOIUrl":"10.1016/j.joule.2024.07.001","url":null,"abstract":"<div><div>Large-scale recycling and regeneration of lithium-ion cathode materials is hindered by the complex mixture of chemistries often present in the waste stream. We outline an efficient process for the separation and regeneration of phases within a blended cathode. We demonstrate the efficacy of this approach using cathode material from a Nissan Leaf end-of-life (40,000 miles) cell. Exploiting the different stabilities of transition metals in acidic media, we demonstrate that ascorbic acid selectively leaches low-value spinel electrode material (LiMn<sub>2</sub>O<sub>4</sub>) from mixed cathode electrode (LiMn<sub>2</sub>O<sub>4</sub>/layered Ni-rich oxide) in minutes, allowing both phases to be effectively recovered separately. This process facilitates upcycling of the Li/Mn content from the resultant leachate solution into higher-value LiNi<sub>x</sub>Mn<sub>y</sub>Co<sub>z</sub>O<sub>2</sub> (NMC) phases, whereas the remaining nickel-rich layered oxide can then be directly regenerated. The method has been extended to other mixtures, with preliminary results illustrating the successful selective leaching of a sodium-ion cathode from a mixture with NMC811.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 10","pages":"Pages 2735-2754"},"PeriodicalIF":38.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141794976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.06.015
Zhiliang Liu , Zhijun Xiong , Shaofei Yang , Ke Fan , Long Jiang , Yuliang Mao , Chaochao Qin , Sibo Li , Longbin Qiu , Jie Zhang , Francis R. Lin , Linfeng Fei , Yong Hua , Jia Yao , Cao Yu , Jian Zhou , Yimu Chen , Hong Zhang , Haitao Huang , Alex K.-Y. Jen , Kai Yao
{"title":"Strained heterojunction enables high-performance, fully textured perovskite/silicon tandem solar cells","authors":"Zhiliang Liu , Zhijun Xiong , Shaofei Yang , Ke Fan , Long Jiang , Yuliang Mao , Chaochao Qin , Sibo Li , Longbin Qiu , Jie Zhang , Francis R. Lin , Linfeng Fei , Yong Hua , Jia Yao , Cao Yu , Jian Zhou , Yimu Chen , Hong Zhang , Haitao Huang , Alex K.-Y. Jen , Kai Yao","doi":"10.1016/j.joule.2024.06.015","DOIUrl":"10.1016/j.joule.2024.06.015","url":null,"abstract":"<div><div><span><span><span>Integrating metal-halide perovskites with the industrially textured Czochralski </span>silicon<span><span> 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 </span>residual strains. Here, we report a strain regulation strategy by forming a 3D/3D perovskite </span></span>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 </span>compressive strain<span> is applied to the upper photoactive 3D perovskite, alleviating its residual tensile stress<span>. 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.</span></span></div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 10","pages":"Pages 2834-2850"},"PeriodicalIF":38.6,"publicationDate":"2024-10-16","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}
JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.07.008
Jianhua Han , Han Xu , Anirudh Sharma , Maxime Babics , Jules Bertrandie , Xunchang Wang , Luis Huerta Hernandez , Yongcao Zhang , Yuanfan Wen , Diego Rosas Villalva , Nicolas Ramos , Sri Harish K. Paleti , Jaime Martin , Fuzong Xu , Joel Troughton , Renqiang Yang , Julien Gorenflot , Frédéric Laquai , Stefaan De Wolf , Derya Baran
{"title":"In situ formation of thermoset matrices for improved stability in organic photovoltaics","authors":"Jianhua Han , Han Xu , Anirudh Sharma , Maxime Babics , Jules Bertrandie , Xunchang Wang , Luis Huerta Hernandez , Yongcao Zhang , Yuanfan Wen , Diego Rosas Villalva , Nicolas Ramos , Sri Harish K. Paleti , Jaime Martin , Fuzong Xu , Joel Troughton , Renqiang Yang , Julien Gorenflot , Frédéric Laquai , Stefaan De Wolf , Derya Baran","doi":"10.1016/j.joule.2024.07.008","DOIUrl":"10.1016/j.joule.2024.07.008","url":null,"abstract":"<div><div>The performance of organic photovoltaics (OPVs) has rapidly increased. Yet, achieving long-term stability in the nano-morphology and thereby sustaining device performance remains challenging. Herein, we show that incorporating <em>in-situ</em>-forming cross-linked thermoset (CLT) matrices into the bulk heterojunction blends is a simple, general, and efficient strategy for high-performing and resilient OPVs. Our simulations and experimental data prove that these high-modulus CLT matrices featuring hydrogen-bonding interactions can freeze the nano-morphology, resulting in long-term thermal and photostable OPV devices. We demonstrate that this approach works efficiently with eight different blends and show that OPV devices can withstand 85°C for 1,000 h without losing performance. Blends with CLT matrices double the energy generated from OPV devices, showing an energy density output of 4,054 mW⋅h cm<sup>−2</sup> over an 11-week operating period under outdoor conditions. This methodology opens avenues for both developing new thermoset networks for OPV and their use in other optoelectronic applications.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 10","pages":"Pages 2883-2902"},"PeriodicalIF":38.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141904253","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}
JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.07.006
Christoph D. Alt , Nadia U.C.B. Müller , Luise M. Riegger , Burak Aktekin , Philip Minnmann , Klaus Peppler , Jürgen Janek
{"title":"Quantifying multiphase SEI growth in sulfide solid electrolytes","authors":"Christoph D. Alt , Nadia U.C.B. Müller , Luise M. Riegger , Burak Aktekin , Philip Minnmann , Klaus Peppler , Jürgen Janek","doi":"10.1016/j.joule.2024.07.006","DOIUrl":"10.1016/j.joule.2024.07.006","url":null,"abstract":"<div><div>The incorporation of lithium metal anodes in solid-state batteries (SSBs) is impeded due to the chemical reduction of sulfide solid electrolytes (SEs) in contact with lithium metal. Growth mode, composition, and microstructure of a few model-type SE interphases (SEIs) are slowly unveiled. The objective of this study is to better understand the transport properties of typical multiphase SEIs by direct reaction of the SE with lithium metal powder. Hence, the composition and conduction properties (<em>σ</em><sub>ion</sub> and <em>σ</em><sub>el</sub>) of synthesized bulk-scale SEI-type material (of Li<sub>6</sub>PS<sub>5</sub>Cl) are analyzed. The kinetic predictions using a Wagner-type diffusion model align well with recent results of electrochemical studies on cell-level multiphase SEIs. Accordingly, these findings enhance the ability to model transport parameters with greater accuracy and contribute to a deeper understanding of SEI growth and kinetics in SSBs. The need to stabilize the Li|SE interface by controlling the partial conductivities of the resulting SEI is emphasized.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 10","pages":"Pages 2755-2776"},"PeriodicalIF":38.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141918670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.09.009
Chong Guo, Lan Xu, Dingxin Wang, Houbing Huang, Weiqi Qian, Huiyu Dan, Chris R. Bowen, Ya Yang
{"title":"Giant pyroelectricity via doping and interface engineering","authors":"Chong Guo, Lan Xu, Dingxin Wang, Houbing Huang, Weiqi Qian, Huiyu Dan, Chris R. Bowen, Ya Yang","doi":"10.1016/j.joule.2024.09.009","DOIUrl":"https://doi.org/10.1016/j.joule.2024.09.009","url":null,"abstract":"Pyroelectricity plays a crucial role in energy harvesting and sensing. High pyroelectric coefficients are the focus of optimizing pyroelectrics. Elevated pyroelectric coefficients not only contribute to the efficiency of energy conversion and signal resolution to be enhanced but also facilitate device miniaturization and cost reduction. However, the pyroelectric coefficients are typically below 1,000 μC/m²K. Here, we achieve a 14-fold enhancement in the pyroelectric coefficient of 8,194 μC/m²K at room temperature for lead magnesium niobate-lead titanate (PMNT) single crystals. This enhancement can be attributed to a synergistic strategy of doping and interface engineering, which enables the coupling of both intrinsic and interface pyroelectricity. Moreover, doping and interface engineering, respectively, contribute to intrinsic pyroelectricity by altering domain structure and polarization and through interface pyroelectricity by introducing polar symmetry. This synergistic strategy provides a framework to design high-performance pyroelectrics for applications in thermal batteries, infrared sensors, and medical imaging devices.","PeriodicalId":343,"journal":{"name":"Joule","volume":"11 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439780","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}
JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.06.018
Oussama Er-raji , Mohamed A.A. Mahmoud , Oliver Fischer , Alexandra J. Ramadan , Dmitry Bogachuk , Alexander Reinholdt , Angelika Schmitt , Bhushan P. Kore , Thomas William Gries , Artem Musiienko , Oliver Schultz-Wittmann , Martin Bivour , Martin Hermle , Martin C. Schubert , Juliane Borchert , Stefan W. Glunz , Patricia S.C. Schulze
{"title":"Tailoring perovskite crystallization and interfacial passivation in efficient, fully textured perovskite silicon tandem solar cells","authors":"Oussama Er-raji , Mohamed A.A. Mahmoud , Oliver Fischer , Alexandra J. Ramadan , Dmitry Bogachuk , Alexander Reinholdt , Angelika Schmitt , Bhushan P. Kore , Thomas William Gries , Artem Musiienko , Oliver Schultz-Wittmann , Martin Bivour , Martin Hermle , Martin C. Schubert , Juliane Borchert , Stefan W. Glunz , Patricia S.C. Schulze","doi":"10.1016/j.joule.2024.06.018","DOIUrl":"10.1016/j.joule.2024.06.018","url":null,"abstract":"<div><div>Fully textured perovskite silicon tandem solar cells are promising for future low-cost photovoltaic deployment. However, the fill factor and open-circuit voltage of these devices are currently limited by the high density of defects at grain boundaries and at interfaces with charge transport layers. To address this, we devise a strategy to simultaneously enhance perovskite crystallization and passivate the perovskite/C<sub>60</sub> interface. By incorporating urea (CO(NH<sub>2</sub>)<sub>2</sub>) as an additive in the solution step of the hybrid evaporation/spin-coating perovskite deposition method, the crystallization kinetics are accelerated, leading to the formation of the desired photoactive phase at room temperature. With that, perovskite films with large grain sizes (>1 μm) and improved optoelectronic quality are formed at low annealing temperatures (100°C). Concurrently, remnant urea molecules are expelled at the perovskite surface, which locally displaces the C<sub>60</sub> layer, thus reducing interfacial non-radiative recombination losses. With this strategy, the resulting tandem solar cells achieve 30.0% power conversion efficiency.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 10","pages":"Pages 2811-2833"},"PeriodicalIF":38.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141726435","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.06.023
Zhibin Li , Ruoyu Wu , Dabo Duan , Xiongjun Liu , Rui Li , Jing Wang , Houwen Chen , Shi-Wei Chen , Yuan Wu , Hui Wang , Suihe Jiang , Xiaobin Zhang , Zhaoping Lu
{"title":"Empowering multicomponent alloys with unique nanostructure for exceptional oxygen evolution performance through self-replenishment","authors":"Zhibin Li , Ruoyu Wu , Dabo Duan , Xiongjun Liu , Rui Li , Jing Wang , Houwen Chen , Shi-Wei Chen , Yuan Wu , Hui Wang , Suihe Jiang , Xiaobin Zhang , Zhaoping Lu","doi":"10.1016/j.joule.2024.06.023","DOIUrl":"10.1016/j.joule.2024.06.023","url":null,"abstract":"<div><div><span><span>Oxygen evolution reaction (OER) catalysts suffer from degradation under harsh oxygen evolution conditions, especially at large </span>current densities<span>, which is a longstanding challenge when developing OER catalysts for industrial applications. Here, we report ultra-stable multicomponent alloys with outstanding OER performance, created by forming two-layered nanostructures<span><span> in noble metal-free multicomponent alloys, which boost activity and stability simultaneously through a counterintuitive parallel-mechanism strategy. The outer multicomponent amorphous </span>oxide layer endows compelling OER activity, while the underneath layer affords dynamic replenishment capability for sustainable performance (working stably at least 1,600 h at 500 mA cm</span></span></span><sup>−2</sup><span><span>) in alkaline electrolytes. More appealing is that the catalyst can be easily revitalized, significantly extending its service durability and reducing its cost. This finding can be applied to develop other cost-efficient catalysts with considerable potential for industrial applications, offering a design paradigm to break the activity-stability trade-off of </span>electrocatalysts.</span></div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 10","pages":"Pages 2920-2937"},"PeriodicalIF":38.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141754633","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}
JoulePub Date : 2024-10-16DOI: 10.1016/j.joule.2024.07.007
Zi-Xuan Wang , Yang Lu , Chen-Zi Zhao , Wen-Ze Huang , Xue-Yan Huang , Wei-Jin Kong , Ling-Xuan Li , Zi-You Wang , Hong Yuan , Jia-Qi Huang , Qiang Zhang
{"title":"Suppressing Li voids in all-solid-state lithium metal batteries through Li diffusion regulation","authors":"Zi-Xuan Wang , Yang Lu , Chen-Zi Zhao , Wen-Ze Huang , Xue-Yan Huang , Wei-Jin Kong , Ling-Xuan Li , Zi-You Wang , Hong Yuan , Jia-Qi Huang , Qiang Zhang","doi":"10.1016/j.joule.2024.07.007","DOIUrl":"10.1016/j.joule.2024.07.007","url":null,"abstract":"<div><div>The application of all-solid-state lithium metal batteries (ASSLMBs) is hampered by the dynamic deterioration of solid-solid contacts. Anodic degradation is primarily attributed to the accumulation of lithium (Li) voids due to the limited Li diffusion abilities of the anodes. Here, a ternary composite Li anode is introduced by comprising carbon materials embedded within the Li-magnesium substrate. This design effectively suppresses the Li void-induced dynamic deterioration of interfacial contact during continuous cycling. The enhanced Li diffusion pathway with accelerated diffusion rate in bulk anode aids in maintaining contact post-Li stripping, therefore mitigating interface damage caused by Li void formation. The ternary composite anode affords an areal capacity of 14.2 mAh cm<sup>−2</sup> with Li utilization rate of 85%. Cooperated with LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> (NCM622) cathodes, the full cells exhibit long-term stability of >300 cycles under room temperature. These findings provide an effective strategy to construct conformal interfaces for high-capacity and long-life ASSLMBs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 10","pages":"Pages 2794-2810"},"PeriodicalIF":38.6,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141974125","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}
JoulePub Date : 2024-10-15DOI: 10.1016/j.joule.2024.09.007
Xinyi Wei, Shivom Sharma, Arthur Waeber, Du Wen, Suhas Nuggehalli Sampathkumar, Manuele Margni, François Maréchal, Jan Van herle
{"title":"Comparative life cycle analysis of electrolyzer technologies for hydrogen production: Manufacturing and operations","authors":"Xinyi Wei, Shivom Sharma, Arthur Waeber, Du Wen, Suhas Nuggehalli Sampathkumar, Manuele Margni, François Maréchal, Jan Van herle","doi":"10.1016/j.joule.2024.09.007","DOIUrl":"https://doi.org/10.1016/j.joule.2024.09.007","url":null,"abstract":"This study conducts a comprehensive life cycle assessment (LCA) of four electrolyzer technologies: alkaline electrolyzer (AEL), proton-exchange membrane (PEM), anion-exchange membrane (AEM), and solid oxide electrolyzer (SOE). It evaluates their environmental impacts across four main categories: climate change (CC), human health (HH), ecosystem quality (EQ), and abiotic stock resources (ASRs). In order to highlight the critical raw materials (CRMs) used in their manufacturing processes, the research identifies potential material replacements and reveals distinct environmental impacts associated with material choices, such as steel in AEL and AEM, platinum in PEM, and nickel in both SOE and AEL. Additionally, we examine the integration of diverse electrolyzer technologies under various scenarios of renewable electricity sources. Together with a sensitivity analysis of regional electricity mixes and the degradation of stacks across different years, the study provides insights into significant opportunities for performance enhancements in emerging electrolyzer technologies.","PeriodicalId":343,"journal":{"name":"Joule","volume":"85 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436360","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}
JoulePub Date : 2024-10-11DOI: 10.1016/j.joule.2024.09.008
Juwon Kim, Si Young Lee, Se-Jun Kim, Bonho Koo, Jinkyu Chung, Danwon Lee, Subin Choi, Jimin Kim, Sungjae Seo, Chihyun Nam, Karl Adrian Gandionco, Gwangsu Bak, Sugeun Jo, Namdong Kim, Hyun-Joon Shin, Keun Hwa Chae, Da Hye Won, Matthew A. Marcus, David A. Shapiro, Shu-Chih Haw, Jongwoo Lim
{"title":"Spatiotemporal active phase evolution for CO2 electrocatalysis","authors":"Juwon Kim, Si Young Lee, Se-Jun Kim, Bonho Koo, Jinkyu Chung, Danwon Lee, Subin Choi, Jimin Kim, Sungjae Seo, Chihyun Nam, Karl Adrian Gandionco, Gwangsu Bak, Sugeun Jo, Namdong Kim, Hyun-Joon Shin, Keun Hwa Chae, Da Hye Won, Matthew A. Marcus, David A. Shapiro, Shu-Chih Haw, Jongwoo Lim","doi":"10.1016/j.joule.2024.09.008","DOIUrl":"https://doi.org/10.1016/j.joule.2024.09.008","url":null,"abstract":"Revealing and redirecting the dynamic evolution of active species in efficient electrochemical CO<sub>2</sub> reduction (ECR) catalysts is challenging. By observing the chemical and morphological evolution in highly efficient ECR catalysts at the nanoscale via <em>operando</em> soft X-ray microscopy, we identified the dynamic transformation of cationic Cu species during operation. The surface Cu<sup>2+</sup> phases, observed during a dynamic phase transformation of Cu(OH)<sub>2</sub>, additionally boost C–C coupling activity beyond the capability of metallic Cu phases. We suggest that copper(II)-carbonate-hydroxide species could dynamically persist under a cathodic environment. By observing the Cu<sup>+</sup> phase during the phase transformation and the formation of surface Cu<sup>2+</sup> species, we were able to electrochemically redirect low-active catalysts into high-active catalysts for C–C coupling. Density functional theory calculations also support that Cu<sup>2+</sup> species could contribute to C–C coupling activity enhancement via ∗CO adsorption energy modulation.","PeriodicalId":343,"journal":{"name":"Joule","volume":"16 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142405463","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}
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号
