钴(Ⅱ)基分子配合物用于光催化二氧化碳还原

doi:10.3866/PKU.WHXB202008068

Abstract

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

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

Figures/Tables 10

Fig 1

Fig 2

Table 1

Co(Ⅱ) complexes as molecular catalysts for photocatalytic CO2 reduction."

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

Table 1

Fig 3

Fig 4

Fig 5

Fig 6

Fig 7

Fig 8

Fig 9

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

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