Boosting Electrochemical Oxygen Reduction to Hydrogen Peroxide Coupled with Organic Oxidation

Overview

Journal Nat Commun

Specialty Biology

Date 2024 Jul 19

PMID 39030230

Authors

Yining Sun

Kui Fan

Jinze Li

Lei Wang

Yusen Yang

Zhenhua Li

Mingfei Shao

Xue Duan

Affiliations

Soon will be listed here.

Abstract

The electrochemical oxygen reduction reaction (ORR) to produce hydrogen peroxide (HO) is appealing due to its sustainability. However, its efficiency is compromised by the competing 4e ORR pathway. In this work, we report a hierarchical carbon nanosheet array electrode with a single-atom Ni catalyst synthesized using organic molecule-intercalated layered double hydroxides as precursors. The electrode exhibits excellent 2e ORR performance under alkaline conditions and achieves HO yield rates of 0.73 mol g h in the H-cell and 5.48 mol g h in the flow cell, outperforming most reported catalysts. The experimental results show that the Ni atoms selectively adsorb O, while carbon nanosheets generate reactive hydrogen species, synergistically enhancing HO production. Furthermore, a coupling reaction system integrating the 2e ORR with ethylene glycol oxidation significantly enhances HO yield rate to 7.30 mol g h while producing valuable glycolic acid. Moreover, we convert alkaline electrolyte containing HO directly into the downstream product sodium perborate to reduce the separation cost further. Techno-economic analysis validates the economic viability of this system.

References

Wang M, Zhang N, Feng Y, Hu Z, Shao Q, Huang X . Partially Pyrolyzed Binary Metal-Organic Framework Nanosheets for Efficient Electrochemical Hydrogen Peroxide Synthesis. Angew Chem Int Ed Engl. 2020; 59(34):14373-14377. DOI: 10.1002/anie.202006422. View

Xie W, Li H, Cui G, Li J, Song Y, Li S . NiSn Atomic Pair on an Integrated Electrode for Synergistic Electrocatalytic CO Reduction. Angew Chem Int Ed Engl. 2020; 60(13):7382-7388. DOI: 10.1002/anie.202014655. View

Zhao Y, Lu X, Fan G, Luan D, Gu X, Lou X . Surface-Exposed Single-Ni Atoms with Potential-Driven Dynamic Behaviors for Highly Efficient Electrocatalytic Oxygen Evolution. Angew Chem Int Ed Engl. 2022; 61(45):e202212542. DOI: 10.1002/anie.202212542. View

Song Y, Ji K, Duan H, Shao M . Hydrogen production coupled with water and organic oxidation based on layered double hydroxides. Exploration (Beijing). 2023; 1(3):20210050. PMC: 10191048. DOI: 10.1002/EXP.20210050. View

Yan Y, Zhou H, Xu S, Yang J, Hao P, Cai X . Electrocatalytic Upcycling of Biomass and Plastic Wastes to Biodegradable Polymer Monomers and Hydrogen Fuel at High Current Densities. J Am Chem Soc. 2023; 145(11):6144-6155. DOI: 10.1021/jacs.2c11861. View

Qorbani M, Sabbah A, Lai Y, Kholimatussadiah S, Quadir S, Huang C . Atomistic insights into highly active reconstructed edges of monolayer 2H-WSe photocatalyst. Nat Commun. 2022; 13(1):1256. PMC: 8913837. DOI: 10.1038/s41467-022-28926-0. View

Zhou Z, Kong Y, Tan H, Huang Q, Wang C, Pei Z . Cation-Vacancy-Enriched Nickel Phosphide for Efficient Electrosynthesis of Hydrogen Peroxides. Adv Mater. 2022; 34(16):e2106541. DOI: 10.1002/adma.202106541. View

Tong Y, Wang L, Hou F, Xue Dou S, Liang J . Electrocatalytic Oxygen Reduction to Produce Hydrogen Peroxide: Rational Design from Single-Atom Catalysts to Devices. Electrochem Energ Rev. 2023; 5(3):7. PMC: 9437407. DOI: 10.1007/s41918-022-00163-5. View

Wang Y, Shi R, Shang L, Waterhouse G, Zhao J, Zhang Q . High-Efficiency Oxygen Reduction to Hydrogen Peroxide Catalyzed by Nickel Single-Atom Catalysts with Tetradentate N O Coordination in a Three-Phase Flow Cell. Angew Chem Int Ed Engl. 2020; 59(31):13057-13062. DOI: 10.1002/anie.202004841. View

10.

Liu J, Gong Z, Yan M, He G, Gong H, Ye G . Electronic Structure Regulation of Single-Atom Catalysts for Electrochemical Oxygen Reduction to H O. Small. 2021; 18(3):e2103824. DOI: 10.1002/smll.202103824. View

11.

Wang Y, Zheng S, Yang W, Zhou R, He Q, Radjenovic P . In situ Raman spectroscopy reveals the structure and dissociation of interfacial water. Nature. 2021; 600(7887):81-85. DOI: 10.1038/s41586-021-04068-z. View

12.

Qi J, Du Y, Yang Q, Jiang N, Li J, Ma Y . Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering. Nat Commun. 2023; 14(1):6263. PMC: 10560254. DOI: 10.1038/s41467-023-41997-x. View

13.

Li X, Tang S, Dou S, Fan H, Choksi T, Wang X . Molecule Confined Isolated Metal Sites Enable the Electrocatalytic Synthesis of Hydrogen Peroxide. Adv Mater. 2021; 34(25):e2104891. DOI: 10.1002/adma.202104891. View

14.

Zhang E, Tao L, An J, Zhang J, Meng L, Zheng X . Engineering the Local Atomic Environments of Indium Single-Atom Catalysts for Efficient Electrochemical Production of Hydrogen Peroxide. Angew Chem Int Ed Engl. 2022; 61(12):e202117347. DOI: 10.1002/anie.202117347. View

15.

Ji K, Xu M, Xu S, Wang Y, Ge R, Hu X . Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural Promoted by a Ru Cu Single-Atom Alloy Catalyst. Angew Chem Int Ed Engl. 2022; 61(37):e202209849. DOI: 10.1002/anie.202209849. View

16.

Zhou H, Ren Y, Li Z, Xu M, Wang Y, Ge R . Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H fuel. Nat Commun. 2021; 12(1):4679. PMC: 8371182. DOI: 10.1038/s41467-021-25048-x. View

17.

Wang Y, Pan Q, Qiao Y, Wang X, Deng D, Zheng F . Layered Metal Oxide Nanosheets with Enhanced Interlayer Space for Electrochemical Deionization. Adv Mater. 2023; 35(15):e2210871. DOI: 10.1002/adma.202210871. View

18.

Bai Y, Wu Y, Zhou X, Ye Y, Nie K, Wang J . Promoting nickel oxidation state transitions in single-layer NiFeB hydroxide nanosheets for efficient oxygen evolution. Nat Commun. 2022; 13(1):6094. PMC: 9568589. DOI: 10.1038/s41467-022-33846-0. View

19.

Jia T, Meng D, Duan R, Ji H, Sheng H, Chen C . Single-Atom Nickel on Carbon Nitride Photocatalyst Achieves Semihydrogenation of Alkynes with Water Protons via Monovalent Nickel. Angew Chem Int Ed Engl. 2023; 62(9):e202216511. DOI: 10.1002/anie.202216511. View

20.

Bu Y, Wang Y, Han G, Zhao Y, Ge X, Li F . Carbon-Based Electrocatalysts for Efficient Hydrogen Peroxide Production. Adv Mater. 2021; 33(49):e2103266. DOI: 10.1002/adma.202103266. View