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Identification of M-NH2 -NH2 Intermediate and Rate Determining Step for Nitrogen Reduction with Bioinspired Sulfur-Bonded FeW Catalyst.

ABSTRACT: The multimetallic sulfur-framework catalytic site of biological nitrogenases allows the efficient conversion of dinitrogen (N2 ) to ammonia (NH3 ) under ambient conditions. Inspired by biological nitrogenases, a bimetallic sulfide material (FeWSx @FeWO4 ) was synthesized as a highly efficient N2 reduction (NRR) catalyst by sulfur substitution of the surface of FeWO4 nanoparticles. Thus prepared FeWSx @FeWO4 catalysts exhibit a relatively high NH3 production rate of 30.2 ug h-1  mg-1 cat and a Faraday efficiency of 16.4 % at -0.45 V versus a reversible hydrogen electrode in a flow cell; these results have been confirmed via purified 15 N2 -isotopic labeling experiments. In situ Raman spectra and hydrazine reduction kinetics analysis revealed that the reduction of undissociated hydrazine intermediates (M-NH2 -NH2 ) on the surface of the bimetallic sulfide catalyst is the rate-determing step for the NRR process. Therefore, this work can provide guidance for elucidating the structure-activity relationship of NRR catalysts.

SUBMITTER: Zhao Y 

PROVIDER: S-EPMC8456964 | biostudies-literature | 2021 Sep

REPOSITORIES: biostudies-literature

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Identification of M-NH<sub>2</sub> -NH<sub>2</sub> Intermediate and Rate Determining Step for Nitrogen Reduction with Bioinspired Sulfur-Bonded FeW Catalyst.

Zhao Yilong Y   Li Fusheng F   Li Wenlong W   Li Yingzheng Y   Liu Chang C   Zhao Ziqi Z   Shan Yu Y   Ji Yongfei Y   Sun Licheng L  

Angewandte Chemie (International ed. in English) 20210806 37

The multimetallic sulfur-framework catalytic site of biological nitrogenases allows the efficient conversion of dinitrogen (N<sub>2</sub> ) to ammonia (NH<sub>3</sub> ) under ambient conditions. Inspired by biological nitrogenases, a bimetallic sulfide material (FeWS<sub>x</sub> @FeWO<sub>4</sub> ) was synthesized as a highly efficient N<sub>2</sub> reduction (NRR) catalyst by sulfur substitution of the surface of FeWO<sub>4</sub> nanoparticles. Thus prepared FeWS<sub>x</sub> @FeWO<sub>4</sub> c  ...[more]

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