二维过渡金属硫属化合物氧还原反应催化剂的研究进展

doi:10.15541/jim20220128

无机材料学报 ›› 2022, Vol. 37 ›› Issue (7): 697-709.DOI: 10.15541/jim20220128 CSTR: 32189.14.10.15541/jim20220128

• 综述 • 下一篇

二维过渡金属硫属化合物氧还原反应催化剂的研究进展

孙炼(), 顾全超, 杨雅萍, 王洪磊, 余金山, 周新贵()

国防科技大学空天科学学院, 新型陶瓷纤维及其复合材料重点实验室, 长沙 410073

收稿日期:2022-03-08 修回日期:2022-04-12 出版日期:2022-07-20 网络出版日期:2022-04-26
通讯作者: 周新贵, 教授. E-mail: zhouxinguilmy@163.com
作者简介:孙炼(1993-), 男, 博士研究生. E-mail: sunlian12@nudt.edu.cn
基金资助:
国家重点研发计划(2018YFB1900603)

Two-dimensional Transition Metal Dichalcogenides for Electrocatalytic Oxygen Reduction Reaction

SUN Lian(), GU Quanchao, YANG Yaping, WANG Honglei, YU Jinshan, ZHOU Xingui()

Science and Technology on Advanced Ceramic Fibers and Composites Laboratory, College of Aerospace Science and Engineering, National University of Defense Technology, Changsha 410073, China

Received:2022-03-08 Revised:2022-04-12 Published:2022-07-20 Online:2022-04-26
Contact: ZHOU Xingui, professor. E-mail: zhouxinguilmy@163.com
About author:SUN Lian (1993-), male, PhD candidate. E-mail: sunlian12@nudt.edu.cn
Supported by:
National Key R&D Plan(2018YFB1900603)

摘要/Abstract

摘要：

氧还原(ORR)反应是燃料电池等清洁能源阴极的关键反应, 其反应动力学复杂, 阴极需使用Pt等贵金属催化剂。然而Pt价格昂贵, 且载体炭黑在高电位环境下稳定性欠佳, 导致电池部件成本高且寿命短。二维过渡金属硫属化合物(2D TMDs)具有高比表面积与可调节的电学性能, 且稳定性强, 有望在维持活性的同时提高燃料电池阴极的耐久性。本文梳理了近年来2D TMDs在ORR催化剂领域的最新研究进展: 首先概述了2D TMDs的结构、性质及ORR反应机理; 其次分析了调控2D TMDs的ORR性能策略, 包括异质元素掺杂、相转变、缺陷工程与应力工程等, 介绍了2D TMDs基异质结构对ORR性能的提升作用; 最后, 针对该领域目前存在的挑战进行展望与总结。

关键词: 氧还原反应, 二维材料, 过渡金属硫属化合物, 电催化, 综述

Abstract:

Oxygen reduction reaction (ORR) is the key reaction in cathode for fuel cells. Because of the sluggish kinetics, platinum (Pt) is widely used as the electrocatalysts for ORR. However, the high cost of Pt and poor stability of carbon black support under high voltage limit the commercialization and durability of fuel cells. Two-dimensional transition metal dichalcogenides (2D TMDs) possess large specific area, tunable electronic structure, and high chemical stability, making them a good candidate for ORR catalysts with high activity and durability. This paper reviews the recent progress of 2D TMDs-based ORR electrocatalysts. First, crystal structure, electronic properties, and ORR reaction mechanism are briefly introduced. Then some strategies for adjusting ORR performance of 2D TMDs are summarized, including heteroatom doping, phase conversion, defect engineering, and strain engineering. Meanwhile, the ORR activity enhancement arising from 2D TMDs-based heterostructures is also analyzed. Finally, perspectives are given for current issues and their possible solutions.

Key words: oxygen reduction reaction, two-dimensional material, transition metal dichalcogenide, electrocatalysis, review

中图分类号:

O614

孙炼, 顾全超, 杨雅萍, 王洪磊, 余金山, 周新贵. 二维过渡金属硫属化合物氧还原反应催化剂的研究进展[J]. 无机材料学报, 2022, 37(7): 697-709.

SUN Lian, GU Quanchao, YANG Yaping, WANG Honglei, YU Jinshan, ZHOU Xingui. Two-dimensional Transition Metal Dichalcogenides for Electrocatalytic Oxygen Reduction Reaction[J]. Journal of Inorganic Materials, 2022, 37(7): 697-709.

图/表 11

图1 2D TMDs的结构与晶型

Fig. 1 Structures and crystal forms of 2D TMDs

图2 (a) 块体结构MoS2, (b) 三层结构MoS2, (c) 双层结构MoS2与(d) 单层结构MoS2经过计算后得到的带隙[26]

Fig. 2 Calculated band structures of (a) bulk MoS2, (b) quadrilayer MoS2, (c) bilayer MoS2, and (d) monolayer MoS2[26]

图3 ORR催化剂的设计理论[3,41]

Fig. 3 Designing strategy for ORR catalysts[3,41] (a) ORR mechanism with blue arrow representing dissociative mechanism, red arrows representing associative mechanism, and purple arrows representing the parts involving both mechanisms[3]; (b) “Volcano plots” showing relationship between oxygen binding energy and maximal activity[41] Colorful figures are available on website

表1 典型2D TMDs层状结构ORR催化剂的性能

Table 1 Properties of typical 2D TMDs-based ORR catalysts

Catalyst	Electrolyte	Onset potential / V (vs. RHE)	Half-wave potential / V (vs. RHE)	Electrons transfer number, n	Ref.
P-MoS₂-0.2	0.1 mol·L^-1 KOH	0.96	0.80	3.60	[45]
I-PdSe₂-50	0.1 mol·L^-1 KOH	-	0.76	3.67	[46]
Ag/MoS₂	0.1 mol·L^-1 KOH	0.90	0.83	3.98	[47]
2H+1T-FeSe@NC	1.0 mol·L^-1 KOH	0.97	0.80	3.90	[48]
O-MoS₂-87	0.1 mol·L^-1 KOH	0.94	0.80	3.49	[49]

图4 2D TMDs的M位掺杂[53,55]

Fig. 4 M-position doping for 2D TMDs[53,55] (a) ORR energy barrier for Pt-MoSe2 with insets showing crystal structures[53] ; (b) TEM images of Pt-SAs/2D TMDs prepared by galvanic replacement[55]

图5 2D TMDs的X位掺杂[45,61]

Fig. 5 X-position doping of 2D TMDs[45,61] (a) ORR polarization curves of P-MoS2 in 0.1 mol·L-1 KOH[45]; (b) Corresponding possible reaction mechanism[61]

图6 由2H-MoS2相转变制备1T-MoS2纳米片的(a)示意图及其(b)在0.1 mol·L-1 KOH的ORR极化曲线与(c)K-L曲线[68]

Fig. 6 (a) Preparative schematic illustration by phase conversion from 2H-MoS2, (b) ORR polarization curves in 0.1 mol·L-1 KOH, and (c) corresponding K-L plots of 1T-MoS2[68] Colorful figures are available on website

图7 2D TMDs的缺陷工程与应力工程调控[46,49,65]

Fig. 7 Defect and strain engineering of 2D TMDs[46,49,65] (a) TEM images and (b) O1s XPS spectra of defected I-PdSe2[46]; (c) Schematic illustration of synthesis of O-MoS2 (d) ORR polarization curves in 0.1 mol·L-1 KOH of O-MoS2[49]; (e) AFM (left) and TEM (middle and right) images of 2H-1T WS2 showing the formation of strain[65]

表2 典型2D TMDs异质结构ORR催化剂的性能

Table 2 Properties of typical 2D TMDs heterostructures-based ORR catalysts

Catalyst	Electrolyte	Onset potential / V (vs. RHE)	Half-wave potential / V (vs. RHE)	Electrons transfer number, n	Ref.
Pt/MoS₂-rGO	0.1 mol·L^-1 HClO₄	0.90	0.80	-	[85]
MoS₂-CNT	0.1 mol·L^-1 KOH	0.65	-	~4.00	[86]
MoS₂/S-PC	0.5 mol·L^-1 H₂SO₄	-	0.86	4.00	[87]
Ni₃S₂/MoS₂	0.1 mol·L^-1 KOH	0.95	0.88	3.99	[88]
hBN-MoS₂	0.1 mol·L^-1 KOH	0.80	0.60	4.00	[89]
FePc-MoS₂	0.1 mol·L^-1 KOH	-	0.89	4.00	[90]

图8 2D TMDs@碳材料异质结ORR催化剂[85,92]

Fig. 8 2D TMDs@carbon materials heterostructure ORR catalysts[85,92] (a) TEM images and (b) activity variations of Pt/MoS2-rGO[85]; (c) SEM image and (d) power density of microbial fuel cells based on N-MoS2/C catalysts[92] Colorful figures are available on website

图9 其它2D TMDs基异质结构ORR催化剂[88⇓-90]

Fig. 9 Other 2D TMDs-based heterostructure ORR catalysts[88⇓-90] (a) TEM image of Ni3S2/MoS2 and (b) corresponding ORR polarization curves in 0.1 mol·L-1 KOH[88]; (c) TEM image of hBN/MoS2 and its (d) ORR durability test[89]; (e) Structure of FePc-MoS2 and (f) its integrated partial density of states IPDOS[90]

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二维过渡金属硫属化合物氧还原反应催化剂的研究进展

Two-dimensional Transition Metal Dichalcogenides for Electrocatalytic Oxygen Reduction Reaction

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