Simulation-guided atomic Ni catalyst with oxygen-enriched coordination environment for H2O2 electrosynthesis coupled with 5-HMF oxidation

• Published in: Chem catalysis Vol. 4; no. 9; p. 101090
• Main Authors: Wang, Jun, Liu, Xiaomei, Ma, Chengbo, Fu, Huanyu, Chen, Shuo, Li, Ning, Li, Yang, Fan, Xiaobin, Peng, Wenchao
• Format: Journal Article
• Language: English
• Published: Elsevier Inc 19.09.2024
• Subjects: coordination microenvironment; coupling system; electrosynthesis oxygen reduction reaction; single-atom catalyst; coordination microenvironment; single-atom catalyst; electrosynthesis oxygen reduction reaction; coupling system; SDG9: Industry, innovation, and infrastructure
• ISSN: 2667-1093; 2667-1093
• DOI: 10.1016/j.checat.2024.101090

The electrosynthesis of H2O2 production via the two-electron oxygen reduction reaction (2e-ORR) has attracted increasing attention. In this work, a novel Ni-N-C single-atom catalyst (SAC) with Ni-N4O1 coordination and a C-O-C synergistic structure is screened out. The corresponding SAC is then synthesized via chelation annealing. During the 2e-ORR test, the Ni-NOC exhibits an H2O2 selectivity of 92.7% at 0.5 V vs. reversible hydrogen electrode (RHE), and the H2O2 production rate can reach 252.91 mmol h−1 g−1 with a TOF of 0.187 s−1, which is among the best Ni-N-C catalysts. In addition, the cathodic 2e-ORR on this SAC is successfully coupled with the anodic oxidation of 5-HMF, and an overpotential of 0.32 V is achieved for 5-HMF oxidation at 50 mA, much smaller than the traditional oxygen evolution reaction (OER) process. Hence, this work provides a promising strategy for designing highly active 2e–ORR SACs as well as a novel coupling system of H2O2 production and 5-HMF electrooxidation. [Display omitted] •Ni-N-C catalyst is screened out by DFT simulation for 2e-ORR•H2O2 selectivity can reach 92.7% when using Ni-NOC as catalyst•Smaller energy consumption can be achieved in coupling craft Considering the intricate coordination structure of central metals, synthesizing desired single-atom catalysts (SACs) with satisfying two-electron oxygen reduction reaction (2e–ORR) performance is a cumbersome and costly task. The novelty of our research lies in the design of SACs with different coordination microenvironments by density functional theory (DFT) screening, which are then synthesized for electrosynthesis of H2O2 via the 2e–ORR. Additionally, by coupling enhanced 5-HMF electrooxidation with the 2e–ORR, the energy-cost anodic oxygen evolution reaction (OER) can be replaced in the valuable chemical production process. The novelty of our research lies in the integration of SACs with different microenvironments and electrocatalytic 2e–ORR efficiency by theoretical screening, guiding significance to reveal the structure-performance relationship of SACs as well as the anode coupling with 5-HMF oxidation.