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自支撑非晶态钴铁磷化物电极同时电催化析氢和聚对苯二甲酸乙二酯塑料重整

Concurrent electrocatalytic hydrogen evolution and polyethylene terephthalate plastics reforming by self-supported amorphous cobalt iron phosphide electrode.

作者信息

Chang Jiuli, Wang Lili, Wu Dapeng, Xu Fang, Jiang Kai, Guo Yuming, Gao Zhiyong

机构信息

School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, Henan Xinxiang 453007, PR China.

Key Laboratory of Yellow River and Huai River Water Environment and Pollution Control, Ministry of Education, Henan Key Laboratory for Environment Pollution Control, International Joint Laboratory on Key Techniques in Water Treatment, Henan Province, School of Environment, Henan Normal University, Henan Xinxiang 453007, PR China.

出版信息

J Colloid Interface Sci. 2024 Feb;655:555-564. doi: 10.1016/j.jcis.2023.11.044. Epub 2023 Nov 9.

Abstract

The electrocatalytic hydrogen evolution reaction (HER) coupled with oxidative transformation of plastics into commodity chemical is a promising tactic to relieve the energy shortage and white pollution problems via sustainable and profitable manner, which necessitates highly active bifunctional catalytic electrode and meticulous construction of electrolysis system. Herein, a self-supported amorphous cobalt iron phosphide onto nickel foam (NF) substrate, labeled as CoFe-P/NF, was prepared by electrodeposition, which served as bifunctional catalytic electrode for alkali hydrogen evolution reaction (HER) and selective electrooxidation of polyethylene terephthalate (PET) plastic hydrolysate toward formate. Benefiting from the abundant catalytic sites within amorphous structure, the interelement synergy and sufficient exposure of catalyst to electrolyte, the self-supported CoFe-P/NF electrode displayed low overpotential (η of 168 mV at current density of J = 100 mA cm), decent stability for HER and fine tolerance to PET monomers. The CoFe-P/NF electrode could also catalyze selective electrooxidation of ethylene glycol (EG) component in PET hydrolysate to formate with high productivity (0.1 mmol cmh) and faradaic efficiency (FE, 90 %) at 1.5 V. The PET hydrolysate electrolysis system based on CoFe-P/NF enabled coproduction of H and value added formate at lower voltage (1.52 V at J = 20 mA cm) and energy consumption (84 % at J = 200 mA cm) relative to water electrolysis. This work showcases the coproduction of H fuel and formate by electrolysis of PET hydrolysate via rational design of bifunctional catalytic electrode. We believe such type of versatile catalytic electrodes can find application scenarios in electrosynthesis of more commodity chemicals and energy devices beyond the case herein.

摘要

将电催化析氢反应(HER)与塑料氧化转化为商品化学品相结合,是一种通过可持续且有利可图的方式缓解能源短缺和白色污染问题的有前景策略,这需要高活性双功能催化电极以及精心构建电解系统。在此,通过电沉积制备了一种负载在泡沫镍(NF)基底上的自支撑非晶态钴铁磷化物,标记为CoFe-P/NF,它用作碱性析氢反应(HER)以及对聚对苯二甲酸乙二酯(PET)塑料水解产物选择性电氧化生成甲酸盐的双功能催化电极。得益于非晶结构中丰富的催化位点、元素间协同作用以及催化剂对电解质的充分暴露,自支撑CoFe-P/NF电极表现出低过电位(在电流密度J = 100 mA cm时η为168 mV)、良好的HER稳定性以及对PET单体的良好耐受性。CoFe-P/NF电极还能在1.5 V下以高生产率(0.1 mmol cm h)和法拉第效率(FE,90%)催化PET水解产物中的乙二醇(EG)组分选择性电氧化生成甲酸盐。基于CoFe-P/NF的PET水解产物电解系统相对于水电解能够在更低电压(在J = 20 mA cm时为1.52 V)和更低能耗(在J = 200 mA cm时为84%)下联产氢气和增值甲酸盐。这项工作通过合理设计双功能催化电极展示了通过电解PET水解产物联产氢气燃料和甲酸盐。我们相信这种多功能催化电极能够在本文所述案例之外的更多商品化学品电合成和能量装置中找到应用场景。

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