Identification of the Highly Active Co-N 4 Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide.

Autor:	Chen S; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China.; Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, 511443 Guangzhou, China., Luo T; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Li X; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Chen K; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Fu J; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Liu K; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Cai C; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Wang Q; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Li H; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Chen Y; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China., Ma C; School of Materials Science and Engineering, Hunan University, Changsha 410082, China., Zhu L; Nanoinstitut München, Fakultät für Physik, Ludwig-Maximilians-Universität München, 80539 München, Germany., Lu YR; National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan., Chan TS; National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan., Zhu M; Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, 511443 Guangzhou, China., Cortés E; Nanoinstitut München, Fakultät für Physik, Ludwig-Maximilians-Universität München, 80539 München, Germany., Liu M; Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physical and Electronics, Central South University, 410083 Changsha, China.
Jazyk:	angličtina
Zdroj:	Journal of the American Chemical Society [J Am Chem Soc] 2022 Aug 17; Vol. 144 (32), pp. 14505-14516. Date of Electronic Publication: 2022 Aug 03.
DOI:	10.1021/jacs.2c01194
Abstrakt:	Electrosynthesis of hydrogen peroxide (H 2 O 2 ) through oxygen reduction reaction (ORR) is an environment-friendly and sustainable route for obtaining a fundamental product in the chemical industry. Co-N 4 single-atom catalysts (SAC) have sparkled attention for being highly active in both 2e - ORR, leading to H 2 O 2 and 4e - ORR, in which H 2 O is the main product. However, there is still a lack of fundamental insights into the structure-function relationship between CoN 4 and the ORR mechanism over this family of catalysts. Here, by combining theoretical simulation and experiments, we unveil that pyrrole-type CoN 4 (Co-N SAC Dp ) is mainly responsible for the 2e - ORR, while pyridine-type CoN 4 catalyzes the 4e - ORR. Indeed, Co-N SAC Dp exhibits a remarkable H 2 O 2 selectivity of 94% and a superb H 2 O 2 yield of 2032 mg for 90 h in a flow cell, outperforming most reported catalysts in acid media. Theoretical analysis and experimental investigations confirm that Co-N SAC Dp ─with weakening O 2 /HOO* interaction─boosts the H 2 O 2 production.
Databáze:	MEDLINE
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