钴(Ⅱ)基分子配合物用于光催化二氧化碳还原

doi:10.3866/PKU.WHXB202008068

物理化学学报 >> 2021, Vol. 37 >> Issue (5): 2008068.doi: 10.3866/PKU.WHXB202008068

所属专题： CO₂还原

钴(Ⅱ)基分子配合物用于光催化二氧化碳还原

张继宏, 钟地长(), 鲁统部()

天津理工大学新能源材料与低碳技术研究院，材料科学与工程学院，天津 300384

收稿日期:2020-08-22 录用日期:2020-09-22 发布日期:2020-09-28
通讯作者: 钟地长,鲁统部 E-mail:dczhong@email.tjut.edu.cn;lutongbu@tjut.edu.cn
作者简介:钟地长，1981年生，天津理工大学教授，博导，2011年于中山大学获得博士学位。主要从事功能配合物的合成及其能源催化方面的研究
鲁统部，1964年生，教授，博导，天津理工大学新能源材料与低碳技术研究院院长。1993年于兰州大学获得博士学位。主要从事人工光合作用催化剂的研究
基金资助:
国家自然科学基金(21931007);国家自然科学基金(21790052);国家自然科学基金(21861001);国家自然科学基金(22071182);111引智计划(D17003);天津市高等教育委员会科技发展基金(2018KJ129)

Co(Ⅱ)-Based Molecular Complexes for Photochemical CO₂ Reduction

Jihong Zhang, Dichang Zhong(), Tongbu Lu()

Institute for New Energy Materials & Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China

Received:2020-08-22 Accepted:2020-09-22 Published:2020-09-28
Contact: Dichang Zhong,Tongbu Lu E-mail:dczhong@email.tjut.edu.cn;lutongbu@tjut.edu.cn
About author:Email: lutongbu@tjut.edu.cn (T.L.); Tel.: +86-22-60214545 (T.L.)
Email: dczhong@email.tjut.edu.cn (D.Z.)
Supported by:
the National Natural Science Foundation of China(21931007);the National Natural Science Foundation of China(21790052);the National Natural Science Foundation of China(21861001);the National Natural Science Foundation of China(22071182);111 Project of China(D17003);the Science & Technology Development Fund of Tianjin Education Commission for Higher Education, China(2018KJ129)

摘要/Abstract

摘要：

利用太阳能将CO₂还原成燃料或高附加值的化工原料，是解决能源危机和气候变暖的理想途径，其中的关键问题是开发高效的催化剂。近年来，非贵金属Co(Ⅱ)配合物作为分子催化剂在光催化CO₂还原方面展现出良好的催化性能。本文按配体的不同种类，系统介绍Co(Ⅱ)配合物分子催化剂在光催化CO₂还原方面的最新研究进展。并在此基础上，重点分析配合物分子结构对催化效率、选择性和稳定性的影响，总结构效关系。最后，针对在光催化CO₂还原中存在的问题，提出了Co(Ⅱ)配合物分子催化剂的设计思路，并对Co(Ⅱ)配合物分子催化剂用于光催化CO₂还原的前景进行了展望。

关键词: 钴(Ⅱ)配合物, 二氧化碳还原, 光催化, 分子催化, 均相催化

Abstract:

Nowadays, more than 85% of the energy is generated by fossil fuels. The excessive utilization of finite fossil fuels has resulted in the crises of energy shortage and global warming caused by greenhouse gas emissions. Researchers have conceived several means for trying to solve these problems, among which the sunlight-driven CO₂ reduction is viewed as a sustainable process that utilizes CO₂ as the raw material to produce chemical fuels, including CO, formate, and CH₄; this method not only realizes the conversion and storage of intermittent solar energy, but also decreases the CO₂ concentration in the atmosphere and alleviates global warming. However, photochemical CO₂ reduction usually undergoes a sluggish process due to the inertness of CO₂. Moreover, the selectivity of the CO₂ reduction reaction is also challenged by the hydrogen evolution reaction, which exhibits faster reaction kinetics. In this context, the rational design and synthesis of efficient and selective catalysts for photochemical CO₂ reduction are major challenges.

Recently, non-noble metal Co(Ⅱ) complexes as molecular catalysts have shown excellent catalytic performances in photocatalytic CO₂ reduction. During the past several decades, significant progress has been achieved in improving the applicability of Co(Ⅱ) complexes for photocatalytic CO₂ reduction. In this review, we systematically report the latest research progress on the use of Co(Ⅱ) complexes in photocatalytic CO₂ reduction. To describe the progress of this research, we characterized the Co(Ⅱ)-based molecular catalysts into four categories according to ligand types, namely: (1) macrocyclic ligands, (2) polypyridine ligands, (3) porphyrin and porphyrin-like ligands, and (4) nonplanar N₄ ligands. The progress of the research on the heterogeneity of Co(Ⅱ) molecular complexes used for photochemical CO₂ reduction was also introduced and discussed. Furthermore, the effects of catalyst structures on catalytic efficiency, selectivity, and stability were particularly summarized and discussed, with the aim of revealing and building the relationship between catalyst structures and catalytic performances to guide the future design and synthesis of Co(Ⅱ) molecular complexes with excellent catalytic performance. Finally, the current challenges and problems in photocatalytic CO₂ reduction were summarized, and several suggestions for designing efficient Co(Ⅱ)-based molecular catalysts for photocatalytic CO₂ reduction were put forward. The trends for the future development of Co(Ⅱ) complex molecular catalysts were also investigated with regard to photocatalytic CO₂ reduction.

Key words: Co(Ⅱ) complexes, Carbon dioxide reduction, Photocatalysis, Molecular catalysis, Homogeneous catalysis

张继宏, 钟地长, 鲁统部. 钴(Ⅱ)基分子配合物用于光催化二氧化碳还原[J]. 物理化学学报, 2021, 37(5), 2008068. doi: 10.3866/PKU.WHXB202008068

Jihong Zhang, Dichang Zhong, Tongbu Lu. Co(Ⅱ)-Based Molecular Complexes for Photochemical CO₂ Reduction[J]. Acta Phys. -Chim. Sin. 2021, 37(5), 2008068. doi: 10.3866/PKU.WHXB202008068

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202008068

https://www.whxb.pku.edu.cn/CN/Y2021/V37/I5/2008068

图/表 10

图1

图2

表1

Co(Ⅱ)配合物分子催化剂光催化CO2还原"

Entry	CAT	PS	SD	Solvent	Light source	Irradiation time (h)	Product (TON)	Quantum yield (%)	Selectivity (%)	Refs.
1	C1 (80 μmol∙L⁻¹)	[Ru(bpy)₃]²⁺	AH⁻	H₂O	daylight lamp	18	CO(22)	–	22	32
2	C2 (80 μmol∙L⁻¹)	[Ru(bpy)₃]²⁺	AH⁻	H₂O	daylight lamp	18	CO(9.6)	–	32	32
3	C3 (80 μmol∙L⁻¹)	[Ru(bpy)₃]²⁺	AH⁻	H₂O	daylight lamp	18	CO (< 3)	–	< 1	32
4	C4 (1.7 mmol∙L⁻¹)	p-terphenyl	TEOA	CH₃CN/MeOH	Hg lamp (λ > 290 nm)	1	CO(10.2) HCOO⁻ (6.7)	15(CO) 10(HCOO⁻)	–	34
5	C4 (2.5 mmol∙L⁻¹)	phenazine	TEA	CH₃CN/MeOH	Hg lamp (λ > 290 nm)	1	HCOO⁻ (5)	7(HCOO⁻)	> 90	35
6	C5 (1.7 mmol∙L⁻¹)	p-terphenyl	TEOA	CH₃CN/MeOH	Hg lamp (λ > 290 nm)	1	CO(5.3) HCOO⁻(3.5)	–	51.6(CO) 34.4(HCOO⁻)	36
7	C6 (1.7 mmol∙L⁻¹)	p-terphenyl	TEOA	CH₃CN/MeOH	Hg lamp (λ > 290 nm)	1	CO(1.0)	–	44	36
8	C7 (1.7 mmol∙L⁻¹)	p-terphenyl	TEOA	CH₃CN/MeOH	Hg lamp (λ > 290 nm)	1	–	–	–	36
9	C8 (1.7 mmol∙L⁻¹)	p-terphenyl	TEOA	CH₃CN/MeOH	Hg lamp (λ > 290 nm)	1	CO(4.9) HCOO⁻(2.5)	–	58.5(CO) 30.4(HCOO⁻)	37
10	C9 (1.7 mmol∙L⁻¹)	p-terphenyl	TEOA	CH₃CN/MeOH	Hg lamp (λ > 290 nm)	1	CO(2.7) HCOO⁻(0.4)	–	30.3(CO) 4.8(HCOO⁻)	36
11	C10 (50 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	CH₃CN	LED (λ > 460 nm)	22	CO(270)	–	97	38
12	C11 (0.5 mmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	DMF	Xe lamp, IR-cut filter	404	CO(8.3)	–	31	39
13	C12 (0.5 mmol∙L⁻¹)	–	TEOA	DMF	Xe lamp (λ > 400 nm)	> 25	CO(3)	–	–	40
14	C13 (0.5 mmol∙L⁻¹)	–	TEOA	DMF	Xe lamp (λ > 400 nm)	> 25	CO(5)	–	–	40
15	C14 (5 μmol∙L⁻¹)	[Ru(bpy)₃]²⁺	BIH	CH₃CN/TEOA	LED (λ = 460 nm)	1.3	CO(2600)	2.8	98	41
16	C14 (5 μmol∙L⁻¹)	purpurin	BIH	DMF	LED (λ = 460 nm)	11	CO(790)	–	95	41
17	C15 (50 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	BIH/TEOA	CH₃CN	LED (λ = 460 nm)	60	CO(221) HCOO⁻(821)	–	75.9(CO)	42
18	C15 (50 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	BIH	CH₃CN/PhOH	LED (λ = 460 nm)	1	CO(829) HCOO⁻(12)	–	96(CO)	42
19	C16 (0.18 mmol∙L⁻¹)	[Ru(bpy)3]²⁺	TEA	CH₃CN/TTA	Xe lamp (λ > 410 nm)	4	CO(3.4) HCOO⁻(1.4)	–	71.4(CO)	43
20	C17 (0.18 mmol∙L⁻¹)	[Ru(bpy)3]²⁺	TEA	CH₃CN/TTA	Xe lamp (λ > 410 nm)	4	CO(5.1)	–	38.9(CO)	43
21	C18 (10 μmol∙L⁻¹)	–	TEA	CH₃CN	Xe lamp (λ > 320 nm)	200	CO+ HCOO⁻(300)	–	–	44
22	C19 (50 μmol∙L⁻¹)	p-terphenyl	TEA	CH₃CN	Xe lamp (λ > 320 nm)	20	CO(62)	–	–	45
23	C20 (40 μmol∙L⁻¹)	p-terphenyl	TEA	CH₃CN	Xe lamp (λ > 310 nm)	6	CO(47.5)	–	–	46
24	C21 (42 μmol∙L⁻¹)	p-terphenyl	TEA	CH₃CN	Xe lamp (λ > 310 nm)	8	CO(50–100)	–	–	45
25	C22 (10 μmol∙L⁻¹)	[Ru(bpy)₃]²⁺	AHˉ	H₂O	Xe lamp (λ > 400 nm)	4	CO(926)	–	82	47
26	C22 (5 μmol∙L⁻¹)	CuPS	AHˉ	H₂O	Xe lamp (λ > 400 nm)	4	CO(1085)	–	90	49
27	C23 (5 μmol∙L⁻¹)	CuPS	AHˉ	H₂O	Xe lamp (λ > 400 nm)	4	CO(2680)	–	77	49
28	C24 (5 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	CH₃CN	LED (λ = 460 nm)	70	CO(953)	–	85	50
29	C25 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	CH₃CN/H₂O	LED (λ = 450 nm)	60	CO(56.9) HCOO⁻(64.2)	–	18.8(CO) 21.2(HCOOˉ)	53
30	C26 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	60	CO(368)	–	95	54
31	C27 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	15	–	–	–	54
32	C28 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	15	CO(13)	–	65	54
33	C29 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	15	–	–	–	54
34	C30 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	12	CO(56)	–	86	55
35	C30 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	48	CO(470)	–	87	55
36	C31 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	12	CO(102)	–	88	55
37	C31 (10 μmol∙L⁻¹)	fac-Ir(ppy)₃	TEA	DMF	LED (λ = 460 nm)	48	CO(403)	–	89	55
38	C32 (2 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(1179)	0.22	97	55
39	C33 (0.05 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(11600)		97	60
40	C34 (0.05 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(1600)	0.007	85	60
41	C35 (0.05 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(12680)	–	97	62
42	C36 (0.05 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(11280)	–	98	62
43	C37 (0.05 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(1600)	–	85	62
44	C38 (2.0 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	12	CO(790)	0.16	98	63
45	C39 (2.0 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	12	CO(1070)	0.22	98	63
46	C40 (2.0 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	12	CO(1330)	0.27	98	63
47	C41 (1.0 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	12	CO(950)	0.19	98	63
48	C42 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(16896)	0.04	98	64
49	C43 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	Blue LED	3	CO(7820)	0.28	87	68
50	C44 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	Blue LED	3	CO(8676)	0.31	83	68
51	C45 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	Blue LED	3	CO(14210)	0.51	95	68
52	C43 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	Blue LED	30	CO(46335) CH₄(2200)	CO(0.17) CH₄(0.03)	CO(90) CH₄(4)	68
53	C44 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	Blue LED	30	CO(27311) CH₄(1766)	CO(0.10) CH₄(0.03)	CO(92) CH₄(6)	68
54	C45 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	Blue LED	30	CO(5641) CH₄(648)	CO(0.02) CH₄(0.01)	CO(63) CH₄(7)	68
55	C46 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(65000)	0.15	98	69
56	C47 (0.025 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(33792)	0.15	98	70
57	C47 (0.5 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O CO2/Ar = 1/9	LED (λ = 450 nm)	10	CO(600)	–	95	70
58	C48 (0.5 μmol∙L⁻¹)	[Ru(phen)₃]²⁺	TEOA	CH₃CN/H₂O	LED (λ = 450 nm)	10	CO(18656)	–	97	70
59	C49 (30 μmol∙L⁻¹)	Ir(ppy)₃	BIH	DMA/TFE	LED (λ = 420 nm)	4	CO(58.4) COOH(55.7)	–	CO(33.2) COOH(31.7)	71

表1

图3

图4

图5

图6

图7

图8

图9

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钴(Ⅱ)基分子配合物用于光催化二氧化碳还原

Co(Ⅱ)-Based Molecular Complexes for Photochemical CO₂ Reduction

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钴(Ⅱ)基分子配合物用于光催化二氧化碳还原

Co(Ⅱ)-Based Molecular Complexes for Photochemical CO2 Reduction

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Co(Ⅱ)-Based Molecular Complexes for Photochemical CO₂ Reduction