Epoxy Group Modified Atomic Zn–N2O2 for H2O2 Electrosynthesis and Sulfide Oxidation

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-10-23 DOI:10.1021/acscatal.4c0472910.1021/acscatal.4c04729
Chengbo Ma, Jun Wang, Xiaomei Liu, Ning Li, Wen Liu, Yang Li, Xiaobin Fan and Wenchao Peng*, 
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Abstract

In this study, zinc single-atom catalysts (SACs) (Zn SACs) with Zn–N2O2 as the coordination shell and the epoxy group (C–O–C) as the second coordination structure are synthesized. The obtained Zn SACs exhibit a high 2e ORR selectivity of >85% in a wide potential window of 0–0.65 V vs RHE and achieve a high generation rate of 828.9 mmol gcat–1 h–1 for H2O2. Experimental and theoretical calculations have confirmed that the second coordination structure of adjacent C–O–C can effectively optimize the adsorption energy of Zn–N2O2 for *OOH and tune the 2e ORR selectivity. In addition, a small onset potential of 0.38 V vs RHE is achieved for sulfides oxidation reaction (SOR) by the obtained Zn SACs. Moreover, a coupled system of anodic SOR and cathodic 2e ORR is fabricated, which can save 45% energy consumption compared to the OER-2e ORR system due to a decreased cell voltage of 2.03 V at 20 mA cm–2. This study provides new bifunctional Zn SACs modified by adjacent C–O–C, which are effective as bifunctional catalysts for electrosynthesis of H2O2 and electro-oxidation of sulfides. These two reactions can be performed together in a coupled system with decreased energy cost and thus should have better application potential.

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用于 H2O2 电合成和硫化物氧化的环氧基改性原子 Zn-N2O2
本研究合成了以 Zn-N2O2 为配位壳、环氧基团(C-O-C)为第二配位结构的锌单原子催化剂(SACs)(Zn SACs)。所获得的 Zn SACs 在 0-0.65 V vs RHE 的宽电位窗口内具有高达 85% 的 2e- ORR 选择性,对 H2O2 的生成率高达 828.9 mmol gcat-1 h-1。实验和理论计算证实,相邻 C-O-C 的第二配位结构能有效优化 Zn-N2O2 对 *OOH 的吸附能,并调节 2e- ORR 的选择性。此外,所获得的 Zn SACs 在硫化物氧化反应(SOR)中的起始电位较小,为 0.38 V vs RHE。此外,还制备了阳极 SOR 和阴极 2e- ORR 耦合系统,与 OER-2e- ORR 系统相比,该系统在 20 mA cm-2 时的电池电压降低了 2.03 V,从而节省了 45% 的能耗。本研究提供了由相邻 C-O-C 修饰的新型双功能 Zn SAC,可有效用作 H2O2 电合成和硫化物电氧化的双功能催化剂。这两个反应可在一个耦合系统中同时进行,且能耗更低,因此具有更好的应用潜力。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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