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The Electrocatalytic Role of Oxygen Vacancy in Nitrate Reduction Reactions.
Li, Hongkun; Ma, Ninggui; Long, Yunchen; Tang, Xinxue; Ou, Weihui; Lyu, Fucong; Liu, Jiahua; Zhou, Binbin; Fan, Jun; Lu, Jian; Li, Yang Yang.
Afiliación
  • Li H; CityU-Shenzhen Futian Research Institute, Shenzhen 518045, China.
  • Ma N; Hong Kong Branch of National Precious Metals Material Engineering Research Centre, City University of Hong Kong, Hong Kong 999077, China.
  • Long Y; Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong 999077, China.
  • Tang X; Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China.
  • Ou W; Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China.
  • Lyu F; Hong Kong Branch of National Precious Metals Material Engineering Research Centre, City University of Hong Kong, Hong Kong 999077, China.
  • Liu J; Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong 999077, China.
  • Zhou B; Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China.
  • Fan J; Hong Kong Branch of National Precious Metals Material Engineering Research Centre, City University of Hong Kong, Hong Kong 999077, China.
  • Lu J; Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong 999077, China.
  • Li YY; Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China.
ACS Appl Mater Interfaces ; 16(35): 46312-46322, 2024 Sep 04.
Article en En | MEDLINE | ID: mdl-39178057
ABSTRACT
Ammonia, with high energy density and easy transportation, holds significant potential to become an integral part of future energy systems. Among tremendous strategies, electrocatalytic ammonia production is no doubt an efficient and eco-friendly method. One particularly intriguing class of electrocatalysts for reducing nitrate to ammonia is transition metal oxides, which have been heavily researched. However, how these catalysts' oxygen vacancy (VO) affects their performance remains elusive. To address this, taking titania (the most important catalyst) as an example, we carried out experimental investigations and simulations. Contrary to the prevailing belief that the concentrated VO would increase the catalytic efficiency of nitrate reduction, it was found that a relatively low level of VO is favorable for maximizing catalytic efficiency. At low cathodic voltages, titania with minimal VO delivered both the highest reduction efficiency and the best selectivity among the different titania samples in this paper. In addition to outlining the merits of lower electron transfer resistance and accelerated reaction dynamics, we also put forth a previously unmentioned factor, the adsorption of hydrogen or the creation of an ordered hydrogen bond network, which put up a hydrogen-rich atmosphere for following nitrate reduction. Further simulation study revealed that within the hydrogen-rich atmosphere isolated VO serves as the ideal active center to enable the lowest energy barriers for the reduction of nitrate into ammonia. These findings offer fresh insights into the working mechanism of oxide-based electrocatalysts for ammonia production.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos