非晶态镍(Ⅲ)基硫化物作为双功能水和尿素氧化阳极电催化剂在含尿素水中制氢

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2022-09-05 DOI:10.1016/j.apcatb.2022.121389
Xin Jia , Hongjun Kang , Xiaoxuan Yang , Yunlong Li , Kai Cui , Xiaohong Wu , Wei Qin , Gang Wu
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引用次数: 54

摘要

设计高性能双功能电催化剂,用于高效析氧反应(OER)和尿素氧化反应(UOR)作为阳极水电解反应,用于含尿素水制氢。本文采用NiCl2(CH3CSNH2)4在室温下水解制备了一种新型非晶Ni(OH)S纳米片电催化剂。从光谱表征和密度泛函理论(DFT)计算可知,Ni(OH)S催化剂中含有富Ni3+相,能显著加速反应动力学。阳极电催化剂表现出优异的OER活性,产生10 mA cm-2,过电压仅为250 mV。当用作UOR阳极时,在1.34 V下可达到10 mA cm-2,比OER低140 mV。值得注意的是,Ni(OH)S/NF阳极表现出良好的双功能UOR和OER活性,与nfe - pba /NF UOR催化剂和典型的RuO2/NF OER催化剂相比,其过电位最低。本研究为双功能OER/UOR电催化剂制备无定形Ni(Ⅲ)基硫化物纳米片提供了一种新策略,对实现含尿素废水高效稳定制氢具有重要意义。
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Amorphous Ni(Ⅲ)-based sulfides as bifunctional water and urea oxidation anode electrocatalysts for hydrogen generation from urea-containing water

It is highly desired to design high-performance bifunctional electrocatalysts for an efficient oxygen evolution reaction (OER) and urea oxidation reaction (UOR) as anode water electrolysis reactions, which can be used for hydrogen production by using urea-containing water. Herein, a novel electrocatalyst composed of amorphous Ni(OH)S nanosheets was prepared by hydrolysis of NiCl2(CH3CSNH2)4 at room temperature. From spectroscopic characterization and density functional theory (DFT) calculations, the Ni(OH)S catalyst contains a Ni3+-rich phase, which can significantly accelerate the reaction kinetics. The anode electrocatalyst shows excellent OER activity, generating 10 mA cm-2 with only 250 mV overpotentials. When employed as a UOR anode, it could reach 10 mA cm-2 at 1.34 V, 140 mV lower than OER. Notably, the Ni(OH)S/NF anode exhibits decent bifunctional UOR and OER activities and presents the lowest overpotentials compared to a NiFe-PBA/NF UOR catalyst and a typical RuO2/NF OER catalyst. This work provides a novel strategy for synthesizing amorphous Ni(Ⅲ)-based sulfides nanosheets for bifunctional OER/UOR electrocatalysts, which is significant for efficient and stable hydrogen production by using urea-containing wastewater.

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来源期刊
Applied Catalysis B: Environmental
Applied Catalysis B: Environmental 环境科学-工程:化工
CiteScore
38.60
自引率
6.30%
发文量
1117
审稿时长
24 days
期刊介绍: Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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