Citation: Wenjuan Tan, Yong Ye, Xiujuan Sun, Bei Liu, Jiajia Zhou, Hailong Liao, Xiulin Wu, Rui Ding, Enhui Liu, Ping Gao. Building P-Poor Ni₂P and P-Rich CoP₃ Heterojunction Structure with Cation Vacancy for Enhanced Electrocatalytic Hydrazine and Urea Oxidation[J]. Acta Physico-Chimica Sinica, ;2024, 40(6): 230605. doi: 10.3866/PKU.WHXB202306054 shu

Building P-Poor Ni₂P and P-Rich CoP₃ Heterojunction Structure with Cation Vacancy for Enhanced Electrocatalytic Hydrazine and Urea Oxidation

Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education, College of Chemistry, Xiangtan University, Xiangtan 411105, Hunan Province, China

Corresponding author: Xiujuan Sun, sunxj594@xtu.edu.cn Bei Liu, liubei@xtu.edu.cn

^†

Received Date: 30 June 2023
Revised Date: 13 August 2023
Accepted Date: 13 August 2023
Available Online: 22 August 2023
Fund Project: the General Project of Education Department of Hunan Province, China 20C1774the Natural Science Foundation of Hunan Province, China 2021JJ40530the Natural Science Foundation of Hunan Province, China 2022JJ40428

Handling hydrazine/urea wastewater through electrochemical oxidation technology (HzOR/UOR) holds significant importance for sewage disposal and nitrogen recycling, as the presence of hydrazine/urea leads to severe environmental issues. On the other hand, hydrazine/urea could potentially serve as a new type of fuel. However, at present, this remains a considerable challenge. The development of a low-cost, highly efficient, and stable electrocatalyst stands as a prerequisite for achieving this goal. In this study, a novel Ni₂P/CoP₃-Zn^vac bimetallic phosphide catalyst is designed and constructed using a hydrothermal-alkali etching-phosphating three-step method. This catalyst integrates P-rich CoP₃, P-poor metallic Ni₂P, and abundant Zn²⁺ cation vacancies into a single structure for HzOR/UOR. Copious P in CoP₃ provides a wealth of negative electrons, which aids in the adsorption of positive reactive intermediates. Meanwhile, P-poor metallic Ni₂P exhibits excellent electrical conductivity, ensuring rapid reaction dynamics. Both physical and electrochemical experiments confirm the successful creation of the Ni₂P/CoP₃-Zn^vac heterojunction, along with the distinctive electron structure of Ni₂P and CoP₃. Electron paramagnetic resonance (EPR) results validate the presence of cation vacancies, which significantly enhance the density of active sites. Consequently, this innovative Ni₂P/CoP₃-Zn^vac heterojunction catalyst displays remarkable electrocatalytic activity, achieving a potential of −47 mV/1.311 V to attain 10 mA∙cm⁻² for HzOR and UOR, respectively. The Tafel slopes of 54.3 and 37.24 mV∙dec⁻¹ for HzOR and UOR are significantly smaller than those of single-phased Ni₂P and CoP₃, as well as the two-phased phosphide without alkali etching. Building upon the excellent HzOR/UOR performance of the Ni₂P/CoP₃-Zn^vac heterojunction, a two-electrode cell for direct hydrazine fuel cells (DHzFC) and direct urea-hydrogen peroxide fuel cells (DUHPFC) is assembled with a Ni₂P/CoP₃-Zn^vac anode. This configuration demonstrates a maximum power density of 229.01 mW∙cm⁻² for DHzFC and 16.22 mW∙cm⁻² for DUHPFC. Moreover, both DHzFC and DUHPFC exhibit exceptional stability for up to 24 h. A homemade aqueous Zn-Hz battery, equipped with a Ni₂P/CoP₃-Zn^vac cathode, further demonstrates its practicality for energy conversion. This work underscores a promising avenue for developing cost-effective and highly stable solutions for UOR and HzOR.
- Ni₂P/CoP₃ heterojunction,
- Cation vacancy,
- Alkaline etching,
- Hydrazine oxidation reaction,
- Urea oxidation reaction
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Building P-Poor Ni2P and P-Rich CoP3 Heterojunction Structure with Cation Vacancy for Enhanced Electrocatalytic Hydrazine and Urea Oxidation

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通讯作者: 陈斌, bchen63@163.com

Building P-Poor Ni₂P and P-Rich CoP₃ Heterojunction Structure with Cation Vacancy for Enhanced Electrocatalytic Hydrazine and Urea Oxidation