构筑富含阳离子缺陷的贫P-Ni2P和富P-CoP3异质结用于增强尿素/肼电催化氧化反应

doi:10.3866/PKU.WHXB202306054

物理化学学报 >> 2024, Vol. 40 >> Issue (6): 2306054.doi: 10.3866/PKU.WHXB202306054

构筑富含阳离子缺陷的贫P-Ni₂P和富P-CoP₃异质结用于增强尿素/肼电催化氧化反应

谭雯娟†, 叶勇†, 孙秀娟*(), 刘备*(), 周佳佳, 廖海龙, 吴秀琳, 丁锐, 刘恩辉, 高平

湘潭大学化学学院, 环境友好与利用教育部重点实验室, 湖南湘潭 411105

收稿日期:2023-06-30 修回日期:2023-08-13 录用日期:2023-08-13 发布日期:2023-11-29
通讯作者: Email: sunxj594@xtu.edu.cn Tel.: +86-136156471 (孙秀娟)liubei@xtu.edu.cn; Tel.: +86-18175631945 (刘备)
作者简介:
^†These authors contributed equally to this work.
基金资助:
湖南省教育厅一般项目(20C1774); 湖南省自然科学基金(2021JJ40530); 湖南省自然科学基金(2022JJ40428)

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

Wenjuan Tan, Yong Ye, Xiujuan Sun*(), Bei Liu*(), Jiajia Zhou, Hailong Liao, Xiulin Wu, Rui Ding, Enhui Liu, Ping Gao

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

Received:2023-06-30 Revised:2023-08-13 Accepted:2023-08-13 Published:2023-11-29
Contact: Email: sunxj594@xtu.edu.cn; Tel.: +86-136156471 (Xiujuan Sun)liubei@xtu.edu.cn; Tel.: +86-18175631945 (Bei Liu)
Supported by:
the General Project of Education Department of Hunan Province, China(20C1774); the Natural Science Foundation of Hunan Province, China(2021JJ40530); the Natural Science Foundation of Hunan Province, China(2022JJ40428)

1. WHXB202306054-SI-16p.pdf(6537KB)

摘要/Abstract

摘要：

废水中存在的肼和尿素会对环境造成严重污染。利用电化学氧化技术处理含肼和尿素的废水，既可以有效处理废水，实现氮循环，又能将肼和尿素作为新型燃料，有助于新能源的发展。然而，目前实现肼氧化(HzOR)和尿素氧化(UOR)的电化学技术仍存在挑战。因此，开发低成本、高效且稳定性好的电催化剂是实现这一技术的先决条件。在本文中，我们采用水热-碱刻蚀-磷化的三步方法，制备了一种富含阳离子缺陷的双金属磷化物Ni₂P/CoP₃催化剂(简称Ni₂P/CoP₃-Zn^vac)，并将其应用于肼氧化和尿素氧化。该催化剂由贫磷的Ni₂P和富磷的CoP₃两种不同性质的磷化物组成。CoP₃中富集的磷含有大量的负电荷，有利于吸附带正电荷的中间物种；而Ni₂P中磷含量较少，金属含量高，具有良好的导电性，可以确保快速的反应动力学。通过物理表征和电化学测试，证实了Ni₂P/CoP₃的成功合成和其独特的电子结构。电子顺磁测试(EPR)证明了阳离子空位的存在，大量的阳离子空位缺陷有助于增加活性位点的数量，从而提升催化性能。因此，该催化剂在肼氧化和尿素氧化方面表现出色。仅需−47 mV (HzOR)和1.311 V(UOR)的电位即可产生10 mA∙cm⁻²的电流密度。Tafel斜率分别为54.3 mV∙dec⁻¹ (HzOR)和37.24 mV∙dec⁻¹ (UOR)。Ni₂P/CoP₃-Zn^vac在HzOR和UOR方面的性能远优于单独的Ni₂P和CoP₃，也优于未经碱刻蚀的镍钴磷化物。基于以上的测试结果，我们将Ni₂P/CoP₃-Zn^vac催化剂应用于直接肼燃料电池(DHzFC)和直接尿素-双氧水燃料电池(DUHPFC)的阳极，测试表明DHzFC和DUHPFC的最大功率密度分别为229.01和16.22 mW∙cm⁻²。更为重要的是，DHzFC和DUHPFC能够稳定工作24 h，性能几乎不衰退。此外，Ni₂P/CoP₃-Zn^vac材料还可应用于自制的锌-肼燃料电池，并展示出良好的实际应用潜力。综上所述，本研究通过一系列方法制备了Ni₂P/CoP₃-Zn^vac催化剂，该催化剂在肼氧化和尿素氧化方面具有优异性能。这项工作为设计高效且稳定性好的肼氧化和尿素氧化电催化剂提供了新的思路。

关键词: Ni₂P/CoP₃异质结, 阳离子空位缺陷, 碱刻蚀, 肼氧化, 尿素氧化

Abstract:

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.

Key words: Ni₂P/CoP₃ heterojunction, Cation vacancy, Alkaline etching, Hydrazine oxidation reaction, Urea oxidation reaction

谭雯娟, 叶勇, 孙秀娟, 刘备, 周佳佳, 廖海龙, 吴秀琳, 丁锐, 刘恩辉, 高平. 构筑富含阳离子缺陷的贫P-Ni₂P和富P-CoP₃异质结用于增强尿素/肼电催化氧化反应[J]. 物理化学学报, 2024, 40(6), 2306054. doi: 10.3866/PKU.WHXB202306054

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 Phys. -Chim. Sin. 2024, 40(6), 2306054. doi: 10.3866/PKU.WHXB202306054

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202306054

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I6/2306054

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构筑富含阳离子缺陷的贫P-Ni₂P和富P-CoP₃异质结用于增强尿素/肼电催化氧化反应

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

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