Highly Boosted Reaction Kinetics in Carbon Dioxide Electroreduction by Surface-Introduced Electronegative Dopants

Zheng Wanzhen; Wang Yu; Shuai LingWang XinyueHe FengLei ChaojunLi ZhongjianYang BinLei LechengYuan ChrisQiu MingHou YangFeng Xinliang

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Highly Boosted Reaction Kinetics in Carbon Dioxide Electroreduction by Surface-Introduced Electronegative Dopants

机译：Highly Boosted Reaction Kinetics in Carbon Dioxide Electroreduction by Surface-Introduced Electronegative Dopants

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Effectively improving the selectivity while reducing the overpotential over the electroreduction of CO2 (CO2ER) has been challenging. Herein, electronegative N atoms and coordinatively unsaturated Ni-N-3 moieties co-anchored carbon nanofiber (Ni-N-3-NCNFs) catalyst via an integrated electrospinning and carbonization strategy are reported. The catalyst exhibits a maximum CO Faradaic efficiency (F.E.) of 96.6%, an onset potential of -0.3 V, and a low Tafel slope of 71 mV dec(-1) along with high stability over 100 h. Aberration corrected scanning transmission electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy identify the atomically dispersed Ni-N-3 sites with Ni atom bonded by three pyridinic N atoms. The existence of abundant electronegative N dopants adjoin the Ni-N-3 centers in Ni-N-3-NCNFs. Theoretical calculations reveal that both, the undercoordinated Ni-N-3 centers and their first neighboring C atoms modified by extra N dopants, display the positive effect on boosting CO2 adsorption and water dissociation processes, thus accelerating the CO2ER kinetics process. Furthermore, a designed Zn-CO2 battery with the cathode of Ni-N-3-NCNFs delivers a maximum power density of 1.05 mW cm(-2) and CO F.E. of 96% during the discharge process, thus providing a promising approach to electric energy output and chemical conversion.

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《Advanced functional materials》 |2021年第15期|2008146.1-2008146.10|共10页
作者
Zheng Wanzhen; Wang Yu; Shuai LingWang XinyueHe FengLei ChaojunLi ZhongjianYang BinLei LechengYuan ChrisQiu MingHou YangFeng Xinliang;
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Zhejiang Univ, Key Lab Biomass Chem Engn, Minist Educ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China|Zhejiang Univ Technol, Coll Environm, Hangzhou 310014, Peoples R China;

Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China;

Cent China Normal Univ, Inst Nanosci & Nanotechnol, Coll Phys Sci & Technol, Wuhan 430079, Peoples R ChinaZhejiang Univ, Key Lab Biomass Chem Engn, Minist Educ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R ChinaZhejiang Univ Technol, Coll Environm, Hangzhou 310014, Peoples R ChinaZhejiang Univ, Key Lab Biomass Chem Engn, Minist Educ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China|Inst Zhejiang Univ, Quzhou 324000, Peoples R ChinaCase Western Reserve Univ, Dept Mech & Aerosp Engn, Cleveland, OH 44106 USATech Univ Dresden, Ctr Adv Elect Dresden Cfaed, D-01062 Dresden, Germany|Tech Univ Dresden, Fac Chem & Food Chem, D-01062 Dresden, Germany;

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正文语种英语
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CO; (2) electroreduction; reaction kinetics; simultaneous effects; unsaturated coordination; Zn; 63743; (2) batteries;

Highly Boosted Reaction Kinetics in Carbon Dioxide Electroreduction by Surface-Introduced Electronegative Dopants

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