Electrocatalytic CO2 Reduction over Pyridinic Nitrogen-Doped Carbon as a Metal-Free Catalyst.

IF 3.9 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Langmuir Pub Date : 2025-10-24 DOI:10.1021/acs.langmuir.5c04434

Chengchen Zhang,Tianxia Liu,Boming Lu

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引用次数: 0

Abstract

The electrochemical reduction of CO2 to CO is an environmentally friendly method of carbon utilization, as it can convert greenhouse gases like CO2 into high value-added chemicals. However, current catalysts suffer from low catalytic activity and poor CO selectivity. Herein, we report a facile and template-free synthesis of nonmetallic nitrogen-doped carbon (N-C) catalysts via the pyrolysis of a conductive carbon black/melamine/polyvinylpyrrolidone precursor. Electrochemical evaluation demonstrated that the N-C 700 catalyst (pyrolyzed at 700 °C) achieved a 94% CO Faraday efficiency at -1.2 V vs RHE, and the CO partial current density was 11 times higher than that of C 700 control. Comprehensive characterization reveals that the pyrolysis temperature critically governs the relative content of multiple nitrogen species (pyridinic, pyrrolic, graphitic) and the concomitant creation of carbon defects. These structural modifications enhanced the CO2-to-CO conversion efficiency, while density functional theory (DFT) calculations further confirmed the significant role of pyridinic nitrogen in promoting CO2 reduction performance.

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吡啶氮掺杂碳作为无金属催化剂的电催化CO2还原。

电化学将CO2还原为CO是一种环保的碳利用方法，因为它可以将CO2等温室气体转化为高附加值的化学物质。然而，现有的催化剂存在催化活性低、CO选择性差的问题。在此，我们报道了一种通过导电炭黑/三聚氰胺/聚乙烯吡咯烷酮前驱体热解制备非金属氮掺杂碳（N-C）催化剂的简便和无模板合成方法。电化学评价表明，在-1.2 V vs RHE条件下，n - c700催化剂（700℃热解）的CO法拉第效率为94%，CO分电流密度是c700对照的11倍。综合表征表明，热解温度对多种氮（吡啶、吡咯、石墨）的相对含量和碳缺陷的产生起着关键的控制作用。这些结构修饰提高了CO2-to- co转化效率，密度泛函理论（DFT）计算进一步证实了吡啶氮对CO2还原性能的显著促进作用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Langmuir 化学-材料科学：综合

CiteScore

6.50

自引率

10.30%

发文量

1464

审稿时长

2.1 months

期刊介绍： Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).