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作者:

Shi, Miao-Miao (Shi, Miao-Miao.) | Bao, Di (Bao, Di.) | Wulan, Ba-Ri (Wulan, Ba-Ri.) | Li, Yong-He (Li, Yong-He.) | Zhang, Yue-Fei (Zhang, Yue-Fei.) (学者:张跃飞) | Yan, Jun-Min (Yan, Jun-Min.) | Jiang, Qing (Jiang, Qing.)

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摘要:

As the N equivalent to N bond in N-2 is one of the strongest bonds in chemistry, the fixation of N-2 to ammonia is a kinetically complex and energetically challenging reaction and, up to now, its synthesis is still heavily relying on energy and capital intensive Haber-Bosch process (150-350 atm, 350-550 degrees C), wherein the input of H-2 and energy are largely derived from fossil fuels and thus result in large amount of CO2 emission. In this paper, it is demonstrated that by using Au sub-nanoclusters (approximate to 0.5 nm) embedded on TiO2 (Au loading is 1.542 wt%), the electrocatalytic N-2 reduction reaction (NRR) is indeed possible at ambient condition. Unexpectedly, NRR with very high and stable production yield (NH3: 21.4 mu g h(-1) mg(cat.)(-1), Faradaic efficiency: 8.11%) and good selectivity is achieved at -0.2 V versus RHE, which is much higher than that of the best results for N-2 fixation under ambient conditions, and even comparable to the yield and activation energy under high temperatures and/or pressures. As isolated precious metal active centers dispersed onto oxide supports provide a well-defined system, the special structure of atomic Au cluster would promote other important reactions besides NRR for water splitting, fuel cells, and other electrochemical devices.

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作者机构:

  • [ 1 ] [Shi, Miao-Miao]Jilin Univ, Dept Mat Sci & Engn, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Peoples R China
  • [ 2 ] [Bao, Di]Jilin Univ, Dept Mat Sci & Engn, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Peoples R China
  • [ 3 ] [Wulan, Ba-Ri]Jilin Univ, Dept Mat Sci & Engn, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Peoples R China
  • [ 4 ] [Yan, Jun-Min]Jilin Univ, Dept Mat Sci & Engn, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Peoples R China
  • [ 5 ] [Jiang, Qing]Jilin Univ, Dept Mat Sci & Engn, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Peoples R China
  • [ 6 ] [Bao, Di]Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Peoples R China
  • [ 7 ] [Li, Yong-He]Beijing Univ Technol, Inst Microstruct & Property Adv Mat, Beijing 100124, Peoples R China
  • [ 8 ] [Zhang, Yue-Fei]Beijing Univ Technol, Inst Microstruct & Property Adv Mat, Beijing 100124, Peoples R China

通讯作者信息:

  • [Yan, Jun-Min]Jilin Univ, Dept Mat Sci & Engn, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Peoples R China

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来源 :

ADVANCED MATERIALS

ISSN: 0935-9648

年份: 2017

期: 17

卷: 29

2 9 . 4 0 0

JCR@2022

ESI学科: MATERIALS SCIENCE;

ESI高被引阀值:169

中科院分区:1

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SCOPUS被引频次: 813

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