{"title":"Poly(ethylenimine)-assisted synthesis of hollow carbon spheres comprising multi-sized Ni species for CO2 electroreduction","authors":"","doi":"10.1016/S1872-2067(24)60087-2","DOIUrl":null,"url":null,"abstract":"<div><p>Electrochemical CO<sub>2</sub> reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion. The development of efficient catalysts with high conductivity and readily accessible active sites for CO<sub>2</sub> electroreduction remains challenging yet indispensable. In this work, a reliable poly(ethyleneimine) (PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles (NPs) (denoted as Ni@NHCS), where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres, but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-N<em>x</em> sites. Benefiting from the unique structural properties of Ni@NHCS, the aggregation and exposure of Ni NPs can be effectively prevented, while the accessibility of abundant catalytically active Ni-N<em>x</em> sites can be ensured. As a result, Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm<sup>–2</sup> and a Faradaic efficiency of 93.0% at −1.0 V <em>vs.</em> RHE, outperforming those of its PEI-free analog. Apart from the excellent activity and selectivity, the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability. The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO<sub>2</sub> reduction. Furthermore, the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.</p></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":15.7000,"publicationDate":"2024-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724600872","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
Abstract
Electrochemical CO2 reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion. The development of efficient catalysts with high conductivity and readily accessible active sites for CO2 electroreduction remains challenging yet indispensable. In this work, a reliable poly(ethyleneimine) (PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles (NPs) (denoted as Ni@NHCS), where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres, but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites. Benefiting from the unique structural properties of Ni@NHCS, the aggregation and exposure of Ni NPs can be effectively prevented, while the accessibility of abundant catalytically active Ni-Nx sites can be ensured. As a result, Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm–2 and a Faradaic efficiency of 93.0% at −1.0 V vs. RHE, outperforming those of its PEI-free analog. Apart from the excellent activity and selectivity, the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability. The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO2 reduction. Furthermore, the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.