A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction
Abstract Atomically dispersed metal–nitrogen sites-anchored carbon materials have been developed as effective catalysts for CO2 electroreduction (CO2ER), but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central metal. Herein, we develop a fami...
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| Format: | Article |
| Language: | English |
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SpringerOpen
2020-05-01
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| Series: | Nano-Micro Letters |
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| Online Access: | http://link.springer.com/article/10.1007/s40820-020-00443-z |
| _version_ | 1818032188343451648 |
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| author | Wanzhen Zheng Feng Chen Qi Zeng Zhongjian Li Bin Yang Lecheng Lei Qinghua Zhang Feng He Xilin Wu Yang Hou |
| author_facet | Wanzhen Zheng Feng Chen Qi Zeng Zhongjian Li Bin Yang Lecheng Lei Qinghua Zhang Feng He Xilin Wu Yang Hou |
| author_sort | Wanzhen Zheng |
| collection | DOAJ |
| description | Abstract Atomically dispersed metal–nitrogen sites-anchored carbon materials have been developed as effective catalysts for CO2 electroreduction (CO2ER), but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central metal. Herein, we develop a family of single metal atom bonded by N atoms anchored on carbons (SAs–M–N–C, M = Fe, Co, Ni, Cu) for CO2ER, which composed of accurate pyrrole-type M–N4 structures with isolated metal atom coordinated by four pyrrolic N atoms. Benefitting from atomically coordinated environment and specific selectivity of M–N4 centers, SAs–Ni–N–C exhibits superior CO2ER performance with onset potential of − 0.3 V, CO Faradaic efficiency (F.E.) of 98.5% at − 0.7 V, along with low Tafel slope of 115 mV dec−1 and superior stability of 50 h, exceeding all the previously reported M–N–C electrocatalysts for CO2-to-CO conversion. Experimental results manifest that the different intrinsic activities of M–N4 structures in SAs–M–N–C result in the corresponding sequence of Ni > Fe > Cu > Co for CO2ER performance. An integrated Zn–CO2 battery with Zn foil and SAs–Ni–N–C is constructed to simultaneously achieve CO2-to-CO conversion and electric energy output, which delivers a peak power density of 1.4 mW cm−2 and maximum CO F.E. of 93.3%. |
| first_indexed | 2024-12-10T06:03:24Z |
| format | Article |
| id | doaj.art-d644bf0803144a538de57cd41837ba20 |
| institution | Directory Open Access Journal |
| issn | 2311-6706 2150-5551 |
| language | English |
| last_indexed | 2024-12-10T06:03:24Z |
| publishDate | 2020-05-01 |
| publisher | SpringerOpen |
| record_format | Article |
| series | Nano-Micro Letters |
| spelling | doaj.art-d644bf0803144a538de57cd41837ba202022-12-22T01:59:46ZengSpringerOpenNano-Micro Letters2311-67062150-55512020-05-0112111210.1007/s40820-020-00443-zA Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 ElectroreductionWanzhen Zheng0Feng Chen1Qi Zeng2Zhongjian Li3Bin Yang4Lecheng Lei5Qinghua Zhang6Feng He7Xilin Wu8Yang Hou9Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang UniversityCollege of Geography and Environmental Science, Zhejiang Normal UniversityKey Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang UniversityKey Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang UniversityKey Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang UniversityKey Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang UniversityZhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang UniversityCollege of Environment, Zhejiang University of TechnologyCollege of Geography and Environmental Science, Zhejiang Normal UniversityKey Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang UniversityAbstract Atomically dispersed metal–nitrogen sites-anchored carbon materials have been developed as effective catalysts for CO2 electroreduction (CO2ER), but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central metal. Herein, we develop a family of single metal atom bonded by N atoms anchored on carbons (SAs–M–N–C, M = Fe, Co, Ni, Cu) for CO2ER, which composed of accurate pyrrole-type M–N4 structures with isolated metal atom coordinated by four pyrrolic N atoms. Benefitting from atomically coordinated environment and specific selectivity of M–N4 centers, SAs–Ni–N–C exhibits superior CO2ER performance with onset potential of − 0.3 V, CO Faradaic efficiency (F.E.) of 98.5% at − 0.7 V, along with low Tafel slope of 115 mV dec−1 and superior stability of 50 h, exceeding all the previously reported M–N–C electrocatalysts for CO2-to-CO conversion. Experimental results manifest that the different intrinsic activities of M–N4 structures in SAs–M–N–C result in the corresponding sequence of Ni > Fe > Cu > Co for CO2ER performance. An integrated Zn–CO2 battery with Zn foil and SAs–Ni–N–C is constructed to simultaneously achieve CO2-to-CO conversion and electric energy output, which delivers a peak power density of 1.4 mW cm−2 and maximum CO F.E. of 93.3%.http://link.springer.com/article/10.1007/s40820-020-00443-zAtomic dispersionPyrrole-type metal–N4 structureCatalytic siteCO2 electroreductionZn–CO2 battery |
| spellingShingle | Wanzhen Zheng Feng Chen Qi Zeng Zhongjian Li Bin Yang Lecheng Lei Qinghua Zhang Feng He Xilin Wu Yang Hou A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction Nano-Micro Letters Atomic dispersion Pyrrole-type metal–N4 structure Catalytic site CO2 electroreduction Zn–CO2 battery |
| title | A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction |
| title_full | A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction |
| title_fullStr | A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction |
| title_full_unstemmed | A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction |
| title_short | A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction |
| title_sort | universal principle to accurately synthesize atomically dispersed metal n4 sites for co2 electroreduction |
| topic | Atomic dispersion Pyrrole-type metal–N4 structure Catalytic site CO2 electroreduction Zn–CO2 battery |
| url | http://link.springer.com/article/10.1007/s40820-020-00443-z |
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