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钯修饰的含钴氮掺杂碳上的高性能电化学CO还原

High performance electrochemical CO reduction over Pd decorated cobalt containing nitrogen doped carbon.

作者信息

Gul Shayan, Nasim Fatima, Iqbal Waheed, Waseem Amir, Nadeem Muhammad Arif

机构信息

Catalysis and Nanomaterials Lab 27, Department of Chemistry, Quaid-i-Azam University Islamabad 45320 Pakistan

Pakistan Academy of Sciences 3-Constitution Avenue Sector G-5/2 Islamabad Pakistan.

出版信息

RSC Adv. 2024 Apr 23;14(19):13017-13026. doi: 10.1039/d4ra01641f. eCollection 2024 Apr 22.

DOI:10.1039/d4ra01641f
PMID:38655488
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11036173/
Abstract

Efficient electrocatalytic CO reduction reaction (eCORR) to various products, such as carbon monoxide (CO), is crucial for mitigating greenhouse gas emissions and enabling renewable energy storage. In this article, we introduce Pd nanoparticles which are deposited over in-house synthesized nitrogen doped tubular carbon (NC) whose ends are blocked with cobalt oxide (CoOx). This composite material is denoted as Pd@CoOx/NC. Among the series of synthesized electrocatalysts, the optimum ratio (Pd@CoOx/NC1) within this category exhibits exceptional performance, manifesting an 81% faradaic efficiency (FE) for CO generation which was quantitatively measured using a gas chromatograph. This remarkable efficiency can be attributed to several scientific factors. Firstly, the presence of Pd nanoparticles provides active sites for CO reduction. Secondly, the NC offer enhanced electrical conductivity and facilitate charge transfer during the reaction. Thirdly, the CoOx capping at the ends of the NC serves to stabilize the catalyst, favoring the formation of CO. The remarkable selectivity of the catalyst is further confirmed by the qualitative CO detection method using PdCl strips. Pd@CoOx/NC1 exhibits a high current density of 55 mA cm and a low overpotential of 251 mV, outperforming Pd decorated multiwalled carbon nanotubes (Pd@MWCNTs) which shows a higher overpotential of 481 mV. Pd@CoOx/NC1 shows long-term stability at different potentials and rapid reaction kinetics. These findings highlight Pd@CoOx/NC1 as promising CO reduction catalysts, with implications for sustainable energy conversion techniques.

摘要

高效电催化将一氧化碳还原反应(eCORR)转化为各种产物,如一氧化碳(CO),对于减少温室气体排放和实现可再生能源存储至关重要。在本文中,我们介绍了沉积在内部合成的氮掺杂管状碳(NC)上的钯纳米颗粒,其端部被氧化钴(CoOx)封闭。这种复合材料被称为Pd@CoOx/NC。在一系列合成的电催化剂中,该类别中的最佳比例(Pd@CoOx/NC1)表现出卓越的性能,使用气相色谱法定量测量显示其生成CO的法拉第效率(FE)为81%。这种显著的效率可归因于几个科学因素。首先,钯纳米颗粒的存在为CO还原提供了活性位点。其次,NC提高了电导率并促进了反应过程中的电荷转移。第三,NC端部的CoOx封端有助于稳定催化剂,有利于CO的形成。使用PdCl试纸的定性CO检测方法进一步证实了催化剂的显著选择性。Pd@CoOx/NC1表现出55 mA cm的高电流密度和251 mV的低过电位,优于钯修饰的多壁碳纳米管(Pd@MWCNTs),后者显示出481 mV的更高过电位。Pd@CoOx/NC1在不同电位下表现出长期稳定性和快速反应动力学。这些发现突出了Pd@CoOx/NC1作为有前景的CO还原催化剂,对可持续能源转换技术具有重要意义。

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本文引用的文献

1
Mechanism of electrocatalytic CO reduction reaction by borophene supported bimetallic catalysts.硼烯负载双金属催化剂催化电还原CO反应的机理
J Colloid Interface Sci. 2024 Apr;659:959-973. doi: 10.1016/j.jcis.2024.01.051. Epub 2024 Jan 12.
2
Metal-organic framework derived single-atom catalysts for electrochemical CO reduction.用于电化学CO还原的金属有机框架衍生单原子催化剂
RSC Adv. 2022 Nov 14;12(50):32518-32525. doi: 10.1039/d2ra06302f. eCollection 2022 Nov 9.
3
A Supported Pd Dual-Atom Site Catalyst for Efficient Electrochemical CO Reduction.
一种用于高效电化学CO还原的负载型钯双原子位点催化剂。
Angew Chem Int Ed Engl. 2021 Jun 7;60(24):13388-13393. doi: 10.1002/anie.202101559. Epub 2021 May 6.
4
Surface Reconstruction of Ultrathin Palladium Nanosheets during Electrocatalytic CO Reduction.电催化一氧化碳还原过程中超薄钯纳米片的表面重构
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5
AgPd nanoparticles for electrocatalytic CO reduction: bimetallic composition-dependent ligand and ensemble effects.用于电催化CO还原的AgPd纳米颗粒:双金属组成依赖性配体和集合效应。
Nanoscale. 2020 Jul 14;12(26):14068-14075. doi: 10.1039/d0nr03203d. Epub 2020 Jun 25.
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Ensemble Effect in Bimetallic Electrocatalysts for CO Reduction.用于CO还原的双金属电催化剂中的协同效应。
J Am Chem Soc. 2019 Oct 23;141(42):16635-16642. doi: 10.1021/jacs.9b05766. Epub 2019 Oct 14.
7
Electrochemical Dealloying-Assisted Surface-Engineered Pd-Based Bifunctional Electrocatalyst for Formic Acid Oxidation and Oxygen Reduction.用于甲酸氧化和氧还原的电化学脱合金辅助表面工程钯基双功能电催化剂
ACS Appl Mater Interfaces. 2019 Apr 17;11(15):14110-14119. doi: 10.1021/acsami.9b00589. Epub 2019 Apr 3.
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Low-Coordinated Edge Sites on Ultrathin Palladium Nanosheets Boost Carbon Dioxide Electroreduction Performance.超薄钯纳米片上的低配位边缘位点提升二氧化碳电还原性能。
Angew Chem Int Ed Engl. 2018 Sep 3;57(36):11544-11548. doi: 10.1002/anie.201806432. Epub 2018 Jul 5.
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Understanding of Strain Effects in the Electrochemical Reduction of CO : Using Pd Nanostructures as an Ideal Platform.理解 CO 的电化学还原中的应变效应:以 Pd 纳米结构为理想平台。
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