具有亲水性的无定形棒状核壳结构NiMoP@CuNWs用于中性介质中高效析氢

doi:10.1016/S1872-2067(24)60086-0

催化学报 ›› 2024, Vol. 63: 154-163.DOI: 10.1016/S1872-2067(24)60086-0

具有亲水性的无定形棒状核壳结构NiMoP@CuNWs用于中性介质中高效析氢

肖佳勇^,¹, 蒋超^,¹, 张辉, 邢卓^*(), 邱明^*(), 余颖

华中师范大学物理科学与技术学院, 湖北武汉 430079

收稿日期:2024-04-11 接受日期:2024-05-24 出版日期:2024-08-18 发布日期:2024-08-19
通讯作者: *电子信箱: xingzhuo@ccnu.edu.cn (邢卓),qium@ccnu.edu.cn (邱明).
作者简介:
¹共同第一作者.
基金资助:
国家重点研发计划(2022YFB3803600);国家自然科学基金(U20A20246);山东省自然科学基金(ZR2020QB133);中央高校基本科研业务费(CCNU22JC017);中央高校基本科研业务费(CCNU24JC013)

Amorphous core-shell NiMoP@CuNWs rod-like structure with hydrophilicity feature for efficient hydrogen production in neutral media

Jiayong Xiao^,¹, Chao Jiang^,¹, Hui Zhang, Zhuo Xing^*(), Ming Qiu^*(), Ying Yu

College of Physical Science and Technology, Central China Normal University, Wuhan 430079, Hubei, China

Received:2024-04-11 Accepted:2024-05-24 Online:2024-08-18 Published:2024-08-19
Contact: *E-mail: xingzhuo@ccnu.edu.cn (Z. Xing), qium@ccnu.edu.cn (M. Qiu).
About author:
¹Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2022YFB3803600);National Natural Science Foundation of China(U20A20246);Shandong Provincial Natural Science Foundation(ZR2020QB133);Fundamental Research Funds for the Central Universities(CCNU22JC017);Fundamental Research Funds for the Central Universities(CCNU24JC013)

1. 附件.zip(35487KB)

摘要/Abstract

摘要：

电化学析氢(HER)是解决能源危机和环境问题的有效手段之一. 目前的研究主要聚焦于强酸或强碱电解质的电解池, 然而这样的工作环境对电解池和电催化剂的长期稳定性构成了挑战. 相比之下, 在中性溶液中电解水制氢则具有环境友好、可持续和性价比高等特点, 更具实际应用价值. 然而, 相较于在酸性或碱性电解液中广泛研究的催化剂, 目前对中性HER催化剂的研究尚显不足. 在HER过程中, 过渡金属磷化物(TMPs)的金属位点和P位点作为氢化物和质子的受体可以发挥协同作用. 其中, 实验和理论研究结果证明, Ni-P化合物在酸性和碱性电解液中具有优异HER性能. 考虑到中性电解液中反应动力学更加缓慢, 还需要额外引入金属位点来优化Ni-P的本征活性. 此外, 调整催化剂的形貌也是提高催化性能的有效方式之一.

本文通过浸渍和电还原法在泡沫铜表面生长出具有高导电能力的铜纳米线作为核芯, 随后通过电沉积法在铜纳米线表面形成由Ni, Mo和P元素组成的无定形壳层, 从而制备出棒状核壳结构的电催化剂(NiMoP@CuNWs/CF). 该催化剂在1.0 mol L^‒1 磷酸盐缓冲盐溶液(PBS)中性溶液的HER性能优于商业Pt/C催化剂, 电流密度为10和100 mA cm^-2时的过电位分别为35和195 mV, Tafel斜率也仅为50 mV dec^-1. 催化剂可以在恒定电流下工作25 h而没有明显的性能衰减, 具有较Pt/C催化剂更好的稳定性. X射线光电子能谱结果表明, Mo元素的成功引入引起了催化剂电子结构的重新分布, 增强了Ni‒P键的强度. 电化学阻抗谱结果表明, Mo的引入大幅度提高了催化剂的电子转移能力. 理论计算结果表明, Mo的引入增强了催化剂的亲水性和水裂解能力, 同时削弱了催化剂表面Ni位点与H原子的结合强度, 促进了H₂产物的脱附. 因而NiMoP@CuNWs/CF相比于NiP@CuNWs/CF的HER性能得到了大幅度提升, 说明Mo的引入优化了Ni-P的析氢活性. 对比各催化剂, 结果表明以铜纳米线核芯作为电沉积的载体相较于直接使用泡沫铜作为载体能够获得更大的电化学活性比表面积, NiMoP@CuNWs/CF是NiMoP/CF的1.61倍, 前者能暴露出更丰富的活性位点. 此外, NiMoP@CuNWs/CF的亲水性也相比于NiMoP/CF得到了明显提升, 促进了电极与电解质溶液的有效接触. 且NiMoP@CuNWs/CF催化剂良好的分散性有利于氢气泡的快速脱附, 在提高反应速率的同时避免了大气泡较大张力对电极的损伤. NiMoP@CuNWs/CF的HER性能和稳定性相较于NiMoP/CF都显著提升, 说明了形貌调控工程的成功.

综上所述, 本文采用简单和低成本的制备方法, 有效地将本征活性调控和形貌调控两种方式相结合, 利用它们在催化性能提升上的协同作用, 成功获得了具有较高催化性能的催化剂. 本研究为中性电解水催化剂的设计提供了新的思路, 也为进一步实现电解海水制氢提供了可能.

关键词: 无定形, 三维核壳结构, 电沉积, 中性电解质, 电催化剂, 析氢反应

Abstract:

Using interface engineering, a highly efficient catalyst with a shell@core structure was successfully synthesized by growing an amorphous material composed of Ni, Mo, and P on Cu nanowires (NiMoP@CuNWs). This catalyst only requires an overpotential of 35 mV to reach a current density of 10 mA cm^-2. The exceptional hydrogen evolution reaction (HER) activity is attributed to the unique amorphous rod-like nature of NiMoP@CuNWs, which possesses a special hydrophilic feature, enhances mass transfer, promotes effective contact between the electrode and electrolyte solution, and exposes more active sites during the catalytic process. Density functional theory revealed that the introduction of Mo weakens the binding strength of the Ni site on the catalyst surface with the H atom and promotes the desorption process of the H₂ product significantly. Owing to its facile synthesis, low cost, and high catalytic performance, this electrocatalyst is a promising option for commercial applications as a water electrolysis catalyst.

Key words: Amorphous, Three-dimensional core-shell, Electrodeposition, Neutral electrolyte, Electrocatalyst, Hydrogen evolution reaction

肖佳勇, 蒋超, 张辉, 邢卓, 邱明, 余颖. 具有亲水性的无定形棒状核壳结构NiMoP@CuNWs用于中性介质中高效析氢[J]. 催化学报, 2024, 63: 154-163.

Jiayong Xiao, Chao Jiang, Hui Zhang, Zhuo Xing, Ming Qiu, Ying Yu. Amorphous core-shell NiMoP@CuNWs rod-like structure with hydrophilicity feature for efficient hydrogen production in neutral media[J]. Chinese Journal of Catalysis, 2024, 63: 154-163.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(24)60086-0

https://www.cjcatal.com/CN/Y2024/V63/I8/154

图/表 5

Fig. 1. (a) Schematic of preparation process of three-dimensional core-shell structure NiMoP@CuNWs/CF, (b-d) SEM images of NiMoP@CuNWs/CF. (e-j) SEM images and SEM-EDS element mapping of NiMoP@CuNWs nanorods.

Fig. 2. TEM (a), HRTEM (b,c) images, SAED pattern (d), corresponding TEM-EDS element mappings (e-h) of NiMoP@CuNW nanorod.

Fig. 3. (a) XPS full spectra of NiMoP@CuNWs/CF and NiP@CuNWs/CF. (b) Ni 2p high-resolution XPS spectra of NiMoP@CuNWs/CF and NiP@CuNWs/CF. (c) Mo 3d high-resolution XPS spectra of NiMoP@CuNWs/CF. (d) P 2p high-resolution XPS maps of NiMoP@CuNWs/CF and NiP@CuNWs/CF.

Fig. 4. (a) HER polarization curves in 1.0 mol L?1 PBS solution. (b) Comparison of overpotential (10 mA cm-2) for NiMoP@CuNWs/CF and various non-precious metal electrocatalysts in neutral electrolyte [3,4,10,14,15,20,50-60]. (c) Tafel slopes of CuNWs/CF, Pt/C/CF, NiMoP@CuNWs/CF, NiMoP/CF and NiP@CuNWs/CF. (d) Linear fitting of the capacitive current densities vs the scan rates of NiMoP@CuNWs/CF, NiMoP/CF, NiP@CuNWs/CF and CuNWs/CF. (e) EIS Nyquist plots of NiMoP@CuNWs/CF, NiMoP/CF, NiP@CuNWs /CF, CuNWs/CF. (f) Long term durability of NiMoP@CuNWs/CF and NiMoP/CF at a current density of 10 mA cm-2.

Fig. 5. (a) Adsorption energy of H2O. (b) PDOSs of Ni-P. (c) Free energy diagram for H adsorption on surfaces of Ni-P and NiMoP. (d) PDOSs of NiMoP.

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具有亲水性的无定形棒状核壳结构NiMoP@CuNWs用于中性介质中高效析氢

Amorphous core-shell NiMoP@CuNWs rod-like structure with hydrophilicity feature for efficient hydrogen production in neutral media

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