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使用ZnCdS/CoP/多壁碳纳米管催化剂通过气液界面介质阻挡放电促进一氧化碳还原生成甲酸盐和甲醛。

Promoting the reduction of CO to formate and formaldehyde via gas-liquid interface dielectric barrier discharge using a ZnCdS/CoP/multiwalled carbon nanotubes catalyst.

作者信息

Li Fangying, Long Yupei, Ma Hao, Qiang Tao, Zhang Guangfeng, Shen Yang, Zeng Lin, Lu Jiani, Cong Yanqing, Jiang Boqiong, Zhang Yi

机构信息

School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China.

Zhejiang E.O. Paton Welding Technology Research Institute, Hangzhou 311200, China.

出版信息

J Colloid Interface Sci. 2022 Sep 15;622:880-891. doi: 10.1016/j.jcis.2022.04.125. Epub 2022 Apr 29.

Abstract

A ZnCdS (ZCS) solid solution was prepared using a hydrothermal method, in which CoP nanowires were added as a co-catalyst and co-deposited with multiwalled carbon nanotubes (MWNTs) on sponge to prepare a series of ZCS/CoP/MWNTs/sponge electrodes. The microstructures of catalysts were analyzed to confirm ZCS and CoP were successfully loaded in MWNTs/sponge. The CO reduction products (formate and formaldehyde) produced via dielectric barrier discharge (DBD) using the different catalysts proved that the introduction of the CoP nanowires co-catalyst can enhance the catalytic activity of ZCS/MWNTs/sponge in the DBD system. Using 10% CoP and a ZCS/CoP concentration of 2.5 g·L, the resulting ZCS/CoP/MWNTs/sponge catalyst exhibited the best catalytic of CO reduction ability toward formate (7894.6 μmol·L) and formaldehyde (308.5 μmol·L) after 60 min of discharge, respectively. The proposed DBD catalytic mechanism for the reduction of CO was analyzed according to the Tafel slope, density functional theory calculations, photocurrent density and plasma reaction process. Furthermore, the application of the DBD catalytic technology for CO capture and reduction was shown to be efficient in a seawater system, and as such, it could be useful for marine CO storage and conversion.

摘要

采用水热法制备了ZnCdS(ZCS)固溶体,其中添加CoP纳米线作为助催化剂,并与多壁碳纳米管(MWNTs)共沉积在海绵上,制备了一系列ZCS/CoP/MWNTs/海绵电极。对催化剂的微观结构进行了分析,以确认ZCS和CoP成功负载在MWNTs/海绵中。使用不同催化剂通过介质阻挡放电(DBD)产生的CO还原产物(甲酸盐和甲醛)证明,引入CoP纳米线助催化剂可以提高ZCS/MWNTs/海绵在DBD系统中的催化活性。使用10%的CoP和2.5 g·L的ZCS/CoP浓度,所得的ZCS/CoP/MWNTs/海绵催化剂在放电60分钟后分别对甲酸盐(7894.6 μmol·L)和甲醛(308.5 μmol·L)表现出最佳的CO还原催化能力。根据塔菲尔斜率、密度泛函理论计算、光电流密度和等离子体反应过程,分析了所提出的DBD催化还原CO的机理。此外,DBD催化技术在海水系统中用于CO捕获和还原的应用被证明是有效的,因此,它可能对海洋CO的储存和转化有用。

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