Journal ArticleDOI
In Situ Phase Separation into Coupled Interfaces for Promoting CO2 Electroreduction to Formate over a Wide Potential Window
Wenbin Wang,Zhitong Wang,Ruoou Yang,Junyuan Duan,Youwen Liu,Anmin Nie,Huiqiao Li,Bao Yu Xia,Tianyou Zhai +8 more
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TLDR
In this paper, the authors showed that the strongly coupled interfaces as real active sites driven the electron self-flow from Sn4+ to Cu+, thereby promoting the delocalized Sn sites to combine HCOO* with H*.Abstract:
Bimetallic sulfides are expected to realize efficient CO2 electroreduction into formate over a wide potential window, however, will undergo in situ structural evolution under the reaction conditions. Therefore, clarifying the structural evolution process, the real active site and the catalytic mechanism appear significance. Here, taking Cu2SnS3 as an example, we unveiled that Cu2SnS3 occurred self-adapted phase separation toward forming the stable SnO2@CuS and SnO2@Cu2O heterojunction during the electrochemical process. Theoretical calculations illustrated that the strongly coupled interfaces as real active sites driven the electron self-flow from Sn4+ to Cu+, thereby promoting the delocalized Sn sites to combine HCOO* with H*. Cu2SnS3 nanosheets achieve over 83.4% formate selectivity in a wide potential range from -0.6 V to -1.1 V. Our findings provide insight into the structural evolution process and performance-enhanced origin of ternary sulfides under the CO2 electroreduction.read more
Citations
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Phase‐Reconfiguration‐Induced NiS/NiFe2O4 Composite for Performance‐Enhanced Zinc−Air Batteries
Zhiyu Shao,Qian Zhu,Yu Sun,Yuanyuan Zhang,Yi-Chao Jiang,Shiqing Deng,Wei Zhang,Keke Huang,Shouhua Feng +8 more
TL;DR: In this article , a NiS/NiFe2O4 composite through a local metal−S coordination at the interface is reported, which is derived from phase reconstruction in the highly defective matrix.
Journal ArticleDOI
In Situ Halogen-Ion Leaching Regulates Multiple Sites on Tandem Catalysts for Efficient CO2 Electroreduction to C2+ Products.
Ruoou Yang,Junyuan Duan,Panpan Dong,Qunlei Wen,Mao Wu,Youwen Liu,Yang Liu,Huiqiao Li,Tianyou Zhai +8 more
TL;DR: In this article , the authors uncovered the interaction of two phases during electrochemical reconstruction by taking AgI-CuO as conceptual tandem catalysts and showed that in situ iodine ion leaching from AgI restrain the entire reduction of CuO to acquiring stable active Cu 0 /Cu + species during CO 2 RR.
Journal ArticleDOI
Engineering a Local Free Water Enriched Microenvironment for Surpassing Platinum Hydrogen Evolution Activity.
Qunlei Wen,Junyuan Duan,Wenbin Wang,Da-Wei Huang,Youwen Liu,Yongliang Shi,Jiakun Fang,Anmin Nie,Huiqiao Li,Tianyou Zhai +9 more
TL;DR: In this article , a local force field was introduced by surface hydroxyl group to engineer the electrochemical microenvironment and enhance alkaline hydrogen evolution activity, showing that the local hydrogen bond induced by the surface group drag 4-coordinated hydrogen-bonded H 2 O molecules across the inner Helmholtz plane to become free HO 2 O and thus continuously supply reactants for catalytic sites.
Journal ArticleDOI
In Situ Chalcogen Leaching Manipulates Reactant Interface toward Efficient Amine Electrooxidation.
Qunlei Wen,Yu-Cheng Lin,Yang Yang,Ruixia Gao,Nanqiu Ouyang,Defang Ding,Youwen Liu,Tianyou Zhai +7 more
TL;DR: In this paper , the authors used operando electrocatalysis variations (i.e., chalcogen leaching) to manipulate the reactant interface toward amine electrooxidation.
Journal ArticleDOI
Synergistic Geometric and Electronic Effects in Bi–Cu Bimetallic Catalysts for CO2 Electroreduction to Formate over a Wide Potential Window
TL;DR: In this article , the electrocatalytic mechanism was identified by combining in situ FT-IR and DFT calculations, which demonstrates that formate prefers to be formed through the HCOO* pathway.
References
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Journal ArticleDOI
Combining theory and experiment in electrocatalysis: Insights into materials design
Zhi Wei Seh,Zhi Wei Seh,Zhi Wei Seh,Jakob Kibsgaard,Jakob Kibsgaard,Jakob Kibsgaard,Colin F. Dickens,Colin F. Dickens,Ib Chorkendorff,Jens K. Nørskov,Jens K. Nørskov,Thomas F. Jaramillo,Thomas F. Jaramillo +12 more
TL;DR: A unified theoretical framework highlights the need for catalyst design strategies that selectively stabilize distinct reaction intermediates relative to each other, and opens up opportunities and approaches to develop higher-performance electrocatalysts for a wide range of reactions.
Journal ArticleDOI
Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte
Stephanie A. Nitopi,Erlend Bertheussen,Søren Bertelsen Scott,Xinyan Liu,Albert K. Engstfeld,Albert K. Engstfeld,Sebastian Horch,Brian Seger,Ifan E. L. Stephens,Ifan E. L. Stephens,Karen Chan,Karen Chan,Christopher Hahn,Christopher Hahn,Jens K. Nørskov,Jens K. Nørskov,Jens K. Nørskov,Thomas F. Jaramillo,Thomas F. Jaramillo,Ib Chorkendorff +19 more
TL;DR: A broad and historical view of different aspects and their complex interplay in CO2R catalysis on Cu is taken, with the purpose of providing new insights, critical evaluations, and guidance to the field with regard to research directions and best practices.
Journal ArticleDOI
What would it take for renewably powered electrosynthesis to displace petrochemical processes
Phil De Luna,Phil De Luna,Phil De Luna,Christopher Hahn,Christopher Hahn,Drew Higgins,Drew Higgins,Drew Higgins,Shaffiq Jaffer,Thomas F. Jaramillo,Thomas F. Jaramillo,Edward H. Sargent +11 more
TL;DR: A comparative analysis of electrocatalyst and carbon emissions assessment of CO2 products such as ethylene, ethanol, and carbon monoxide shows that electrocatalytic production has the potential to yield the greatest reduction in carbon emissions, provided that a steady supply of clean electricity is available.
Journal ArticleDOI
Tailoring the d-Band Centers Enables Co4N Nanosheets To Be Highly Active for Hydrogen Evolution Catalysis
Zhiyan Chen,Zhiyan Chen,Yao Song,Yao Song,Jinyan Cai,Xusheng Zheng,Dongdong Han,Yishang Wu,Yishang Wu,Yipeng Zang,Shuwen Niu,Yun Liu,Junfa Zhu,Xiaojing Liu,Gongming Wang +14 more
TL;DR: This work successfully endow Co4 N with prominent HER catalytic capability by tailoring the positions of the d-band center through transition-metal doping, which could provide valuable insights into the design of other catalysts for HER and beyond.
Journal ArticleDOI
Electrochemical CO2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design.
Golam Kibria,Jonathan P. Edwards,Christine M. Gabardo,Cao-Thang Dinh,Ali Seifitokaldani,David Sinton,Edward H. Sargent +6 more
TL;DR: A techno-economic analysis is presented with the goal of identifying maximally profitable products and the performance targets that must be met to ensure economic viability-metrics that include current density, Faradaic efficiency, energy efficiency, and stability.