Surface-confined self-reconstruction to sulfate-terminated ultrathin layers on NiMo3S4 toward biomass molecule electro-oxidation

Wu，Tong1,2; Xu，Zian3,4; Wang，Xunlu1; Luo，Mengjia1,2; Xia，Yu3; Zhang，Xingcai5; Li，Jiantao6; Liu，Jie1; Wang，Jiacheng1,2,8; Wang，Hsing Lin3; Huang，Fuqiang1,2,7

2023-04-01

10.1016/j.apcatb.2022.122126

APPLIED CATALYSIS B-ENVIRONMENTAL   Impact Factor & Quartile

0926-3373

1873-3883

Developing high-performance anode electrocatalysts is desirable in electrocatalytic energy devices powered by sustainable electricity. Compared to water oxidation using Ni-based anodes, electro-oxidation upgrading of biomass molecule with larger size lacks dynamics driving due to increased thickness and decreased electron transfer kinetics of insulating NiOOH amorphous layer (>50 nm) from uncontrollable in-depth reconstruction. Herein, a self-confined surface reconstruction strategy is proposed to construct ∼5 nm-thick NiOOH layers on NiMoS with superior activity and stability for 5-hydroxymethylfurfural oxidation reaction (HMFOR). In-situ high-valence Mo-O coordination and sulfate-terminated anion groups effectively prevent in-depth surface oxidation, leading to the ultra-thin active layers with increased electron transfer kinetics. The surface self-reconstructed NiMoS (NiMoS-R) exhibits nearly 100% of HMF conversion, FDCA selectivity and Faradaic efficiency, much better than sulfate-modified NiOOH and pure NiOOH. Moreover, a paired electrolyzer of NiMoS-R||NiMoS for HMFOR||HER is also assembled with an ultralow voltage of 1.414 V at 10 mA cm.

5-Hydroxymethylfurfural Electrocatalysis Surface self-reconstruction Theoretical calculation

EI ; SCI

English

Others

Program of Shanghai Academic Research Leader[20XD1424300];National Natural Science Foundation of China[52072389];National Natural Science Foundation of China[92163117];

Chemistry ; Engineering

Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical

WOS:000890468200002

ELSEVIER

20224513091358

Anodes ; Electrocatalysts ; Electron transitions ; Electrooxidation ; Indium compounds ; Molecules ; Nickel compounds ; Sulfur compounds

Electron Tubes:714.1 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Atomic and Molecular Physics:931.3

CHEMISTRY

2-s2.0-85141446667

Scopus

1.State Key Laboratory of High Performance Ceramics and Superfine Microstructure,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai,200050,China
2.Center of Materials Science and Optoelectronics Engineering,University of Chinese Academy of Sciences,Beijing,100049,China
3.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,Guangdong Province,518055,China
4.Institute of Applied Physics and Materials Engineering,University of Macau,China
5.John A. Paulson School of Engineering and Applied Sciences,Harvard University,Cambridge,02138,United States
6.State Key Laboratory of Advanced Technology for Materials Synthesis and processing,Wuhan University of Technology,Wuhan,Hubei,430070,China
7.State Key Laboratory of Rare Earth Materials Chemistry and Applications,College of Chemistry and Molecular Engineering,Peking University,Beijing,100871,China
8.School of Materials Science and Engineering,Taizhou University,Taizhou,318000,China

Wu，Tong,Xu，Zian,Wang，Xunlu,et al. Surface-confined self-reconstruction to sulfate-terminated ultrathin layers on NiMo3S4 toward biomass molecule electro-oxidation[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2023,323.

Wu，Tong.,Xu，Zian.,Wang，Xunlu.,Luo，Mengjia.,Xia，Yu.,...&Huang，Fuqiang.(2023).Surface-confined self-reconstruction to sulfate-terminated ultrathin layers on NiMo3S4 toward biomass molecule electro-oxidation.APPLIED CATALYSIS B-ENVIRONMENTAL,323.

Wu，Tong,et al."Surface-confined self-reconstruction to sulfate-terminated ultrathin layers on NiMo3S4 toward biomass molecule electro-oxidation".APPLIED CATALYSIS B-ENVIRONMENTAL 323(2023).