Библиографическое описание:BCN-Encapsulated Nano-nickel Synergistically Promotes Ambient Electrochemical Dinitrogen Reduction / X. Zhao [et al.]. - Текст : непосредственный // ACS Appl Mater Interfaces. - 2020. - Vol. 12, Is. 28. - P. 31419-31430. - Cited Reference Count: 68. - This work was financially supported by the Fundamental Research Funds for the Central Universities (no. 2042016HF1054) and Wuhan University Experiment Technology Project Funding (no. WHU-2016-SYJS-06). This work was also supported by the Olle Engkvist Byggmastare Foundation (contract no. 189-0223), the Air Force Office of Scientific Research (contract FA-9550-18-1-0032), and the Ministry of Education and Science of Ukraine (project no. 0117U003908). The quantum-chemical calculations were performed with computational resources provided by the National Supercomputer Centre at Linkoping University (Sweden) through the project "Multiphysics Modeling of Molecular Materials" SNIC 2019-2-41. We are grateful to Pei Zhang and Bichao Xu of the Core Facility and Technical Support, Wuhan Institute of Virology, for their technical support in transmission electron microscopy., Fundamental Research Funds for the Central UniversitiesFundamental Research Funds for the Central Universities. 2042016HF1054. - Wuhan University Experiment Technology Project Funding. WHU-2016-SYJS-06. - Olle Engkvist Byggmastare Foundation. 189-0223. - Air Force Office of Scientific ResearchUnited States Department of DefenseAir Force Office of Scientific Research (AFOSR). FA-9550-18-1-0032. - Ministry of Education and Science of Ukraine. 0117U003908. - ISSN ISSN- 194, DOI 10.1021/acsami.0c06649.
Аннотация:The electricity provided by solar or wind power can drive nitrogen in the atmosphere, combining with ubiquitous water to form ammonia, and distributed production methods can alleviate the irreversible damage to the environment caused by the energy-intensive Haber-Bosch process. Here, we have designed a novel Ni-doped BCN heterojunction (S/M-BOPs-1) as a catalyst for the electrochemical nitrogen reduction reaction (NRR). The ammonia yield rate and Faraday efficiency in NRR driven by S/M-BOPs-1 reach up to 16.72 μg-1 h-1 cm-2 and 13.06%, respectively. Moreover, S/M-BOPs-1 still maintains high NRR activity and excellent stability after recycling for eight times and long-time operation of 12 h. Using density functional theory calculations, we reveal a possible NRR path for N2 to NH3 on Ni, BCN, and the S/M-BOPs-1 composite surfaces. The interaction between the BCN matrix and Ni nanoparticles promotes a synergetic effect for the electrochemical NRR efficiency due to the partial electron transfer from the Ni particles to BCN that inhibits hydrogen evolution reaction and decreases the rate-determining step on Ni surfaces toward NRR by ∼1.5 times. Therefore, efficient NRR performance can be achieved by tuning the electronic properties of non-noble metals via the formation of a heterointerface.
Держатель оригинала документа:College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China, Division of Theoretical Chemistry and Biology, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of TechnologyStockholm 10691, Sweden, Department of Science and Innovations, Siberian Federal University, 79 Svobodny Avenue, Krasnoyarsk, 660041, Russian Federation, Department of Chemistry and Nanomaterials Science, Bohdan Khmelnytsky National UniversityCherkasy 18031, Ukraine, College of Chemistry and Chemical Engineering, Henan University, Kaifeng, Henan 475004, China, Department Key Laboratory of Flexible Electronics (KLOFE) & Institute of Advanced Materials (IAM), Nanjing Tech University, Nanjing, 211800, China, National Demonstration Center for Experimental Chemistry, Wuhan University, Wuhan, 430072, China, Engineering Research Center of Organosilicon Compounds & Materials, Ministry of Education, Wuhan University, Wuhan, 430072, China
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