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作者:

Cheng, Xing (Cheng, Xing.) | Xiao, Bo (Xiao, Bo.) | Chen, Yanhui (Chen, Yanhui.) | Wang, Yueshuai (Wang, Yueshuai.) | Zheng, Lirong (Zheng, Lirong.) | Lu, Yue (Lu, Yue.) | Li, Hongyi (Li, Hongyi.) | Chen, Ge (Chen, Ge.) (学者:陈戈)

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EI Scopus SCIE

摘要:

Developing oxide supports for stabilizing single-atom catalysts enables more flexibility for tuning the electronic metal-support interactions (EMSIs) toward better catalytic activities. However, due to the electronegativity of oxygen anions, single-metal atoms often remain positively charged in these oxide supports and are poor at binding hydrogen species for the hydrogen evolution reaction (HER). Here, we report a ligand charge donation-acquisition balance strategy via an amorphous TiBxOy support to tune the EMSIs, which lead to the boosted HER mass activity of a single Pt atom catalyst. Based on spectroscopic characterizations, we found that Pt single atoms preferentially bonded with nearly neutral B atoms originating from TiB2-like species in the Ti-B-O framework rather than O anions. Density functional theory calculations reveal that due to the charge-transfer balance between B-O and B-Pt, the nucleophilicity of Pt was tuned to an optimum state, with an ideal hydrogen binding energy that benefits the HER. As a result, this Pt/TiBxOy catalyst achieves a high HER mass activity (37.8 A mg(-1) Pt) and a turnover frequency (33.2 H-2 s(-1) Pt site(-1)) at an overpotential of 50 mV in an acid medium, outperforming commercial Pt/C by a factor of 34 and 33, respectively.

关键词:

single atom charge transfer amorphous support hydrogen evolution reaction electronic metal-support interactions

作者机构:

  • [ 1 ] [Cheng, Xing]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 2 ] [Xiao, Bo]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 3 ] [Chen, Ge]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 4 ] [Chen, Yanhui]Beijing Univ Technol, Fac Mat & Mfg, Beijing 100124, Peoples R China
  • [ 5 ] [Wang, Yueshuai]Beijing Univ Technol, Fac Mat & Mfg, Beijing 100124, Peoples R China
  • [ 6 ] [Lu, Yue]Beijing Univ Technol, Fac Mat & Mfg, Beijing 100124, Peoples R China
  • [ 7 ] [Li, Hongyi]Beijing Univ Technol, Fac Mat & Mfg, Beijing 100124, Peoples R China
  • [ 8 ] [Zheng, Lirong]Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China

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来源 :

ACS CATALYSIS

ISSN: 2155-5435

年份: 2022

期: 10

卷: 12

页码: 5970-5978

1 2 . 9

JCR@2022

1 2 . 9 0 0

JCR@2022

ESI学科: CHEMISTRY;

ESI高被引阀值:53

JCR分区:1

中科院分区:1

被引次数:

WoS核心集被引频次: 34

SCOPUS被引频次: 32

ESI高被引论文在榜: 0 展开所有

万方被引频次:

中文被引频次:

近30日浏览量: 6

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