Amorphous low-coordinated cobalt sulphide nanosheet electrode for electrochemically synthesizing hydrogen peroxide in acid media

被引:31
作者
Chen, Zhenglin [1 ]
Liu, Guangzhen [2 ]
Cao, Wenjing [2 ]
Yang, Lixia [2 ]
Zhang, Longshuai [2 ]
Zhang, Shuqu [2 ]
Zou, Jianping [2 ]
Song, Renjie [2 ]
Fan, Wenhong [1 ]
Luo, Shenglian [1 ,2 ]
Dionysiou, Dionysios D. [3 ]
机构
[1] Beihang Univ, Sch Space & Environm, Beijing 100191, Peoples R China
[2] Nanchang Hangkong Univ, Key Lab Jiangxi Prov Persistent Pollutants Control, Nanchang 330063, Peoples R China
[3] Univ Cincinnati, Dept Chem & Environm Engn, Environm Engn & Sci Program, Cincinnati, OH 45221 USA
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2023年 / 334卷
基金
中国国家自然科学基金;
关键词
Low-coordination; H2O2; 2e(-) oxygen reduction reaction; CoSx; Amorphous; OXYGEN REDUCTION; EVOLUTION; CATALYSTS; H2O2; GENERATION; ELECTROCATALYSTS;
D O I
10.1016/j.apcatb.2023.122825
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
This study investigates in-depth the local atomic environment-property relationship of amorphous low-coordination catalysts toward the 2e(-) oxygen reduction reaction (ORR). Here, an ethanol-assisted slow nucleation strategy was adopted to flexibly regulate the intrinsic activity of CoSx nanostructures for efficient 2e(-) ORR by oriented control the coordination number of Co. When Co and S form Co-S-4 coordination structures, the CuNW@CoS4 exhibits an ultra-low overpotential (0.018 V) with 93 % H2O2 selectivity, and 91 % Faraday efficiency in acidic media at 0.1 V-RHE. Furthermore, thus produced H2O2 satisfies in-situ organic pollutants degradation by electro-Fenton. XAS and DFT calculations unveil the S-induced forming of abundant low-coordinated Co atoms as active sites in Co-S4, validating that a favorable D-band energy level of Co center can weaken the OOH* adsorption for accelerating the H2O2 production kinetics. This work is anticipated to enlighten the rational design of high-performance ORR catalysts for practically feasible H2O2 electrosynthesis toward wastewater remediation.
引用
收藏
页数:11
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