金属-有机框架原位转化合成无定形Fe基双金属氢氧化物催化剂催化析氧反应性能

doi:10.1016/S1872-2067(20)63741-X

催化学报 ›› 2021, Vol. 42 ›› Issue (8): 1370-1378.DOI: 10.1016/S1872-2067(20)63741-X

金属-有机框架原位转化合成无定形Fe基双金属氢氧化物催化剂催化析氧反应性能

许友^a^,^b, 任凯丽^a, 徐蓉^b^,^*()

^a浙江工业大学化学工程学院, 绿色化学合成技术国家重点实验室培育基地, 浙江杭州 310014, 中国
^b南洋理工大学化学与生物医学工程学院, 新加坡 637459, 新加坡

收稿日期:2020-08-31 接受日期:2020-10-22 出版日期:2021-08-18 发布日期:2020-12-10
通讯作者: 徐蓉
作者简介:^*. 电子信箱: rxu@ntu.edu.sg
基金资助:
南洋理工大学和国家自然科学基金(21701141)

In situ formation of amorphous Fe-based bimetallic hydroxides from metal-organic frameworks as efficient oxygen evolution catalysts

You Xu^a^,^b, Kaili Ren^a, Rong Xu^b^,^*()

^aState Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, Zhejiang, China
^bSchool of Chemical & Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore;

Received:2020-08-31 Accepted:2020-10-22 Online:2021-08-18 Published:2020-12-10
Contact: Rong Xu
About author:^*. E-mail: rxu@ntu.edu.sg
Supported by:
This work was supported by the Nanyang Technological University and the National Natural Science Foundation of China(21701141)

摘要/Abstract

摘要：

传统化石能源的大量消耗使得能源短缺和环境污染等问题日益严峻. 社会的可持续发展需要进行能源结构调整, 寻求清洁、可再生的替代能源已迫在眉睫. 氢能作为一种可再生能源, 其热值高, 燃烧产物无污染, 是未来最理想的能源形式之一. 水裂解制氢是公认的未来清洁制氢的一种有效途径. 然而, 无论是电催化或光催化水裂解反应, 析氧反应都是关键的半反应. 因其复杂的四电子过程导致动力学缓慢, 使得析氧半反应成为水裂解反应的瓶颈. 长久以来, 贵金属Ir和Ru基材料是被广泛研究的高活性的析氧催化剂. 然而高成本和低储量极大地限制了它们的大规模工业化应用. 因此, 开发高效、储量丰富的析氧催化剂, 意义重大但仍充满挑战性.
本文考察了一种简便而有效的合成策略, 在碱性水溶液条件下, 成功实现将一系列Fe基金属有机框架(MOF)前驱物原位转化为无定形Fe基双金属氢氧化物纳米结构. 这些由MOF前驱物转化得到的氢氧化物纳米结构保留了前驱体纳米棒的宏观形貌, 由许多超细的无定形纳米颗粒(平均粒径小于10 nm)构成, 在催化反应中可以提供丰富的催化活性位, 相邻的纳米颗粒之间紧密接触, 有利于电子在催化活性位之间传递. 以玻碳电极作为基底, 通过组分优化得到的NiFe-OH-0.75催化剂样品在电催化析氧反应中仅需270 mV的过电位便可达到10 mA cm ^‒2的电流密度, Tafel斜率为39 mV dec ^‒1. 将催化剂负载到三维泡沫镍基底上时, 由于电极基底导电性提升以及传质增加, 在10 mA cm ^-2的电流密度所需的过电位可以降低到235 mV, Tafel斜率为37 mV dec ^-1, 并且表现出较好的稳定性. 同时, 本文进一步证实这些无定形氢氧化物可以用作助催化剂, 与合适的光敏剂结合, 实现有效的光催化水氧化反应. 在KH₂PO₄-K₂HPO₄缓冲溶液(pH = 9)体系中, 以[Ru(2,2’-bipyridine)₃]Cl₂为光敏剂, Na₂S₂O₈为电子受体, 由CoFe-MIL-0.75前驱体转化所得到的CoFe-OH-0.75助催化剂表现出更优越的光催化产氧性能, 产氧效率可达59.6%. 本文结果可以为其他基于MOF及其相关衍生材料的制备提供新思路.

关键词: 双金属氢氧化物, 电催化, 金属有机框架, 析氧反应, 光催化

Abstract:

Oxygen evolution from water driven by electrocatalysis or photocatalysis poses a significant challenge as it requires the use of efficient electro-/photo-catalysts to drive the four-electron oxygen evolution reaction (OER). Herein, we report the development of an effective strategy for the in situ chemical transformation of Fe-based bimetallic MIL-88 metal-organic frameworks (MOFs) into corresponding bimetallic hydroxides, which are composed of amorphous ultrasmall nanoparticles and afford an abundance of catalytically active sites. Optimized MOF-derived NiFe-OH-0.75 catalyst coated on glassy carbon electrodes achieved a current density of 10 mA cm ^‒2 in the electrocatalytic OER with a small overpotential of 270 mV, which could be decreased to 235 mV when loading the catalysts on a nickel foam substrate. Moreover, these MOF-derived Fe-based bimetallic hydroxides can be used as efficient cocatalysts when combined with suitable photosensitizers for photocatalytic water oxidation.

Key words: Bimetallic hydroxides, Electrocatalysis, Metal-organic frameworks, Oxygen evolution reaction, Photocatalysis

许友, 任凯丽, 徐蓉. 金属-有机框架原位转化合成无定形Fe基双金属氢氧化物催化剂催化析氧反应性能[J]. 催化学报, 2021, 42(8): 1370-1378.

You Xu, Kaili Ren, Rong Xu. In situ formation of amorphous Fe-based bimetallic hydroxides from metal-organic frameworks as efficient oxygen evolution catalysts[J]. Chinese Journal of Catalysis, 2021, 42(8): 1370-1378.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(20)63741-X

https://www.cjcatal.com/CN/Y2021/V42/I8/1370

图/表 8

Scheme 1. Schematic illustration of the preparation of the MOF-derived Fe-based bimetallic hydroxides.

Fig. 1. SEM (a) and TEM (b) images of the NiFe-MIL-0.75. SEM (c,d), TEM (e), HRTEM (f), and HAADF-STEM (g) and elemental mapping images of the as-converted NiFe-OH-0.75.

Fig. 2. XRD patterns (a) and Raman spectra (b) of NiFe-MIL-0.75 and the as-converted NiFe-OH-0.75; High-resolution Fe 2p (c) and high-resolution Ni 2p (d) XPS spectra of NiFe-OH-0.75.

Fig. 3. SEM image (a) of the CoFe-MIL-0.75. The inset of (a) is the TEM image of CoFe-MIL-0.75. SEM (b), TEM (c), HRTEM (d), and HAADF- STEM (e) images and element mapping images of the CoFe-OH-0.75. The inset of (d) is the SAED pattern of the CoFe-OH-0.75.

Fig. 4. OER polarization curves (a,c) and Tafel plots (b,d) for the various catalysts loaded on different electrode substrates. (a,b) GC electrode; (c,d) nickel foam electrode.

Fig. 5. CV curves at various scan rates and capacitive current densities of the NiFe-OH-0.75 decorated GC electrode (a,c) and NiFe-OH-0.75(H) decorated GC electrode (b,d).

Fig. 6. Time-dependent potential curve (a) and time-dependent current density curve (b) (without iR compensation) of the NiFe-OH-0.75/Ni foam electrode.

Fig. 7. Time-dependent photocatalytic O2 evolution over various cocatalysts by coupling with a [Ru(bpy)3]Cl2 photosensitizer.

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金属-有机框架原位转化合成无定形Fe基双金属氢氧化物催化剂催化析氧反应性能

In situ formation of amorphous Fe-based bimetallic hydroxides from metal-organic frameworks as efficient oxygen evolution catalysts

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