Your browser doesn't support javascript.
loading
Selective electrochemical reduction of nitric oxide to hydroxylamine by atomically dispersed iron catalyst.
Kim, Dong Hyun; Ringe, Stefan; Kim, Haesol; Kim, Sejun; Kim, Bupmo; Bae, Geunsu; Oh, Hyung-Suk; Jaouen, Frédéric; Kim, Wooyul; Kim, Hyungjun; Choi, Chang Hyuck.
Afiliación
  • Kim DH; School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju, Republic of Korea.
  • Ringe S; Department of Energy Science and Engineering, Daegu Gyeongbuk Institute of Science and Technology, Daegu, Republic of Korea.
  • Kim H; School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju, Republic of Korea.
  • Kim S; Department of Chemistry, Korea Advanced Institute of Science and Technology, Daejeon, Republic of Korea.
  • Kim B; Department of Chemical Engineering, Pohang University of Science and Technology, Pohang, Republic of Korea.
  • Bae G; School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju, Republic of Korea.
  • Oh HS; Clean Energy Research Center, Korea Institute of Science and Technology, Seoul, Republic of Korea.
  • Jaouen F; ICGM, Université de Montpellier, CNRS, ENSCM, Montpellier, France.
  • Kim W; Department of Chemical and Biological Engineering, Sookmyung Women's University, Seoul, Republic of Korea. wkim@sookmyung.ac.kr.
  • Kim H; Department of Chemistry, Korea Advanced Institute of Science and Technology, Daejeon, Republic of Korea. linus16@kaist.ac.kr.
  • Choi CH; School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju, Republic of Korea. chchoi@gist.ac.kr.
Nat Commun ; 12(1): 1856, 2021 03 25.
Article en En | MEDLINE | ID: mdl-33767159
Electrocatalytic conversion of nitrogen oxides to value-added chemicals is a promising strategy for mitigating the human-caused unbalance of the global nitrogen-cycle, but controlling product selectivity remains a great challenge. Here we show iron-nitrogen-doped carbon as an efficient and durable electrocatalyst for selective nitric oxide reduction into hydroxylamine. Using in operando spectroscopic techniques, the catalytic site is identified as isolated ferrous moieties, at which the rate for hydroxylamine production increases in a super-Nernstian way upon pH decrease. Computational multiscale modelling attributes the origin of unconventional pH dependence to the redox active (non-innocent) property of NO. This makes the rate-limiting NO adsorbate state more sensitive to surface charge which varies with the pH-dependent overpotential. Guided by these fundamental insights, we achieve a Faradaic efficiency of 71% and an unprecedented production rate of 215 µmol cm-2 h-1 at a short-circuit mode in a flow-type fuel cell without significant catalytic deactivation over 50 h operation.
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2021 Tipo del documento: Article Pais de publicación: Reino Unido
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2021 Tipo del documento: Article Pais de publicación: Reino Unido