Donor-Acceptor Nanocarbon Ensembles to Boost Metal-Free All-pH Hydrogen Evolution Catalysis by Combined Surface and Dual Electronic Modulation

被引:59
作者
Yang, Meijia [1 ]
Zhang, You [1 ]
Jian, Junhua [1 ]
Fang, Long [1 ]
Li, Jing [1 ]
Fang, Zhengsong [1 ]
Yuan, Zhongke [1 ]
Dai, Liming [2 ]
Chen, Xudong [1 ]
Yu, Dingshan [1 ]
机构
[1] Sun Yat Sen Univ, Key Lab Polymer Composite & Funct Mat, Key Lab High Performance Polymer Based Composites, Sch Chem,Minist Educ, Guangzhou 510275, Guangdong, Peoples R China
[2] Case Western Reserve Univ, Dept Macromol Sci & Engn, Cleveland, OH 44106 USA
关键词
electrocatalysis; hydrogen evolution; electronic modulation; energy conversion; N-doped carbon; NITROGEN-DOPED GRAPHENE; OXYGEN REDUCTION; CARBON NANOTUBES; FREE ELECTROCATALYSTS; NANOPOROUS GRAPHENE; CHARGE-TRANSFER; H-2; PRODUCTION; EFFICIENT; CO; NANOSHEETS;
D O I
10.1002/anie.201907826
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A combined surface and dual electronic modulation strategy is used to realize metal-free all-pH catalysis towards the hydrogen evolution reaction (HER) by coupling a N-doped carbon framework (MHCF, electron acceptors) derived from MOFs with higher-Fermi-level pure carbon nanotubes (CNTs, electron donors), followed by surface modification with carboxyl-group-rich polymers. Although the three constituents are inactive, as-assembled ternary membranes yield superior HER performance with low overpotentials and high durability (<= 5 % activity loss over 100 h) at all pH values. The C adjacent to pyrrolic N in MHCF is the most active site and the induced directional interfacial electron transfer from CNTs to MHCF coupled with N-driven intramolecular electron transfer in MHCF optimizes Gibbs free energy for hydrogen adsorption (Delta G(H*)) near zero, while the polymer modulation enables local H+ enrichment in acidic media and enhanced water adsorption and activation in neutral and basic media.
引用
收藏
页码:16217 / 16222
页数:6
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