原位合成氧化镍硼/石墨炔杂化材料用于提高光/电催化产氢性能

doi:10.1016/S1872-2067(20)63601-4

催化学报 ›› 2021, Vol. 42 ›› Issue (8): 1379-1386.DOI: 10.1016/S1872-2067(20)63601-4

原位合成氧化镍硼/石墨炔杂化材料用于提高光/电催化产氢性能

殷学鹏, 罗舒文, 唐上峰, 卢秀利^*, 鲁统部^#

天津理工大学材料科学与工程学院新能源材料与低碳技术研究院, 材料微结构教育部国际合作联合实验室, 天津300384
天津理工大学材料科学与工程学院新能源材料与低碳技术研究院, 材料微结构教育部国际合作联合实验室, 天津 300384

收稿日期:2020-01-06 接受日期:2020-01-06 出版日期:2021-08-18 发布日期:2020-11-23
通讯作者: 卢秀利,鲁统部
作者简介:^#. lutongbu@tjut.edu.cn
^*. 电话/传真: (022)60215704; 电子信箱: luxiuli@email.tjut.edu.cn
第一联系人：
^† 共同第一作者
基金资助:
天津市教委科研计划项目(2018KJ129)

In situ synthesis of a nickel boron oxide/graphdiyne hybrid for enhanced photo/electrocatalytic H₂ evolution

Xue-Peng Yin, Shu-Wen Luo, Shang-Feng Tang, Xiu-Li Lu^*, Tong-Bu Lu^#

MOE International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Material Science & Engineering, Tianjin University of Technology, Tianjin 300384, China

Received:2020-01-06 Accepted:2020-01-06 Online:2021-08-18 Published:2020-11-23
Contact: Xiu-Li Lu,Tong-Bu Lu
About author:^#E-mail: lutongbu@tjut.edu.cn
^*. Tel/Fax: +86-22-60215704; E-mail: luxiuli@email.tjut.edu.cn
First author contact:
^† These authors contributed equally to this work
Supported by:
This work was supported by the Science and Technology Development Fund of Tianjin Education Commission for Higher Education(2018KJ129)

摘要/Abstract

摘要：

当今世界面临严峻的能源紧缺和环境污染问题, 发展高效无污染的清洁能源替代传统化石能源成为近几十年科研工作者的研究热点. 其中, 氢能由于具有高燃烧值和产物无污染等优点成为理想的替代能源. 光/电催化水分解产生氢气是最有效的制氢方法之一. 目前, 高活性的产氢催化剂仍以贵金属为主, 但贵金属价格高昂和稀缺性等限制了其大规模应用, 因此, 开发和设计廉价、高效的非贵金属产氢催化剂变得尤为重要. 为了提高非贵金属催化剂的催化活性, 基于非贵金属的复合材料的构建被广泛研究. 例如, 通过非贵金属和碳材料的复合, 能够提高比表面积和电子传输速率, 优化活性位点的电子结构, 从而提高催化活性.
石墨炔(GDY)作为一种新兴碳材料, 由sp ²-和sp-杂化碳共同组成. 由于GDY具有高度π共轭结构, 大的比表面积和独特的双炔键, 可作为载体与非贵金属离子相互作用形成复合材料, 制备高效产氢催化剂. 基于此, 本文在室温下原位合成了强耦合相互作用的氧化镍硼/石墨炔(NiB_i/GDY)催化剂, 并将其应用于光/电催化产氢反应. 在光催化产氢反应中, 采用曙红为光敏剂, 三乙醇胺为牺牲剂, 可见光下NiB_i/GDY的光催化产氢速率可达4.54 mmol g ^-1 h ^-1, 产氢速率分别是氧化镍硼/石墨烯(NiB_i/graphene)和NiB_i的2.9倍和4.5倍. 此外, NiB_i/GDY在1.0 M KOH溶液中也表现出良好电催化产氢性能, 电流密度为400 mA/cm ²时其过电位为478.0 mV, 低于商业铂碳(505.3 mV@400 mA/cm ²). NiB_i/GDY在光/电催化产氢实验中表现出的较好催化性能可归因于NiB_i和GDY之间强耦合相互作用对NiB_i电子结构的优化. 上述研究结果表明, 石墨炔可作为理想载体制备高效的光/电催化剂, 同时本文为设计高效稳定的非贵金属产氢催化剂提供了一定的借鉴意义.

关键词: 石墨炔, 杂化材料, 光/电催化剂, 水分解反应, 氢析出

Abstract:

Developing highly active catalysts for photo/electrocatalytic water splitting is an attractive strategy to produce H₂ as a renewable energy source. In this study, a new nickel boron oxide/graphdiyne (NiB_i/GDY) hybrid catalyst was prepared by a facile synthetic approach. Benefitting from the strong electron donating ability of graphdiyne, NiB_i/GDY showed an optimized electronic structure containing lower valence nickel atoms and demonstrated improved catalytic performance. As expected, NiB_i/GDY displayed a high photocatalytic H₂ evolution rate of 4.54 mmol g ^‒1 h ^‒1, 2.9 and 4.5 times higher than those of NiB_i/graphene and NiB_i, respectively. NiB_i/GDY also displayed outstanding electrocatalytic H₂ evolution activity in 1.0 M KOH solution, with a current density of 400 mA/cm ² at an overpotential of 478.0 mV, which is lower than that of commercial Pt/C (505.3 mV@400 mA/cm ²). This work demonstrates that GDY is an ideal support for the development of highly active catalysts for photo/electrocatalytic H₂ evolution.

Key words: Graphdiyne, Hybrid material, Photo/electrocatalyst, Water splitting reaction, H₂ evolution

殷学鹏, 罗舒文, 唐上峰, 卢秀利, 鲁统部. 原位合成氧化镍硼/石墨炔杂化材料用于提高光/电催化产氢性能[J]. 催化学报, 2021, 42(8): 1379-1386.

Xue-Peng Yin, Shu-Wen Luo, Shang-Feng Tang, Xiu-Li Lu, Tong-Bu Lu. In situ synthesis of a nickel boron oxide/graphdiyne hybrid for enhanced photo/electrocatalytic H₂ evolution[J]. Chinese Journal of Catalysis, 2021, 42(8): 1379-1386.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(20)63601-4

https://www.cjcatal.com/CN/Y2021/V42/I8/1379

图/表 5

Fig. 1. SEM images of GDY (a) and NiBi/GDY (b); TEM images of NiBi/GDY (c,d) and NiBi (e); The insets of d and e are the corresponding SAED images of NiBi/GDY and NiBi, respectively; (f) EDS mapping images of NiBi/GDY.

Scheme 1. The in situ growth of NiBi on GDY at room temperature.

Fig. 2. (a) XRD patterns of GDY and NiBi/GDY, (b) Raman spectra of GDY and NiBi/GDY, (c) Ni 2p, and (d) B 1s XPS patterns of NiBi and NiBi/GDY.

Fig. 3. (a) Time dependence of photocatalytic H2 generation using NiBi/GDY, NiBi/graphene, NiBi, and GDY catalysts (Reaction conditions: 2 mg catalyst, 3 mg Eosin Y, 5 mL aqueous solution containing 10 vol% TEOA, Xe-lamp (300 W, λ > 400 nm)). (b) Photocatalytic activity recycling test for NiBi/GDY. (c) Steady-state photoluminescence spectra of NiBi/GDY, NiBi/graphene, and NiBi. (d) Time-resolved fluorescence decay spectra of NiBi/GDY, NiBi/graphene, and NiBi.

Fig. 4. (a) LSV curves of electrochemical HER activities. (b) Electrochemical surface area (ECSA) measurements of NiBi/GDY, NiBi/graphene, and NiBi vs. scan rate. (c) Nyquist plots for NiBi, NiBi/graphene, and NiBi/GDY samples at ?0.2 V vs. RHE. (d) Polarization curves of NiBi/GDY obtained initially and after 2000 cycles (inset: time dependence of the cathodic current density of NiBi/GDY over 40 h).

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原位合成氧化镍硼/石墨炔杂化材料用于提高光/电催化产氢性能

In situ synthesis of a nickel boron oxide/graphdiyne hybrid for enhanced photo/electrocatalytic H₂ evolution

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原位合成氧化镍硼/石墨炔杂化材料用于提高光/电催化产氢性能

In situ synthesis of a nickel boron oxide/graphdiyne hybrid for enhanced photo/electrocatalytic H2 evolution

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In situ synthesis of a nickel boron oxide/graphdiyne hybrid for enhanced photo/electrocatalytic H₂ evolution