聚合物半导体光催化合成过氧化氢：光氧化还原中心的空间分离和协同利用

doi:10.3866/PKU.WHXB202301001

Abstract

Abstract:

The photocatalytic synthesis of hydrogen peroxide using earth-abundant water and/or O₂ as raw materials and solar energy as the sole energy input is an attractive route to achieving a carbon-neutral future. In particular, semiconducting polymer photocatalysts have piqued the interest of researchers working on the photocatalytic synthesis of H₂O₂ because their bandgap structures, reactivation sites, and components are easily tunable at the molecular level. However, there are two major challenges: 1) the photoredox centers are difficult to separate and recombine easily, resulting in low reactivity in the photocatalytic production of H₂O₂, and 2) the low utilization rate of the redox centers. In several cases, only one side of the redox center is used for the photocatalytic synthesis of H₂O₂, while the other side typically reacts with a sacrificial agent. In this review, we provide a timely survey of recent advances in the spatial separation and synergistic utilization of photoredox centers for photocatalytic H₂O₂ production. The key aspect for achieving spatial separation of the redox centers is to engineer electron donor-acceptor (D-A) units on a single photocatalyst, such as by incorporating atomically dispersed metals into the polymer frameworks to build metal-organic D-A units or constructing all-organic D-A units. Depending on the photocatalytic behavior of the redox centers, the synergistic utilization of photoredox centers can be classified into three major reaction models: 1) the oxygen reduction reaction (ORR) combined with the oxidative production of chemicals; 2) the water oxidation reaction (WOR) combined with the reductive production of chemicals; and 3) the ORR combined with the WOR. Based on this, the regulation modes, characteristics, catalytic mechanisms, and reaction pathways to overcome the two challenges of efficient H₂O₂ production are summarized and discussed. Finally, we demonstrate efficient photocatalytic H₂O₂ production and provide prospects and challenges for the photocatalytic production of H₂O₂ using photoredox centers.

Key words: H₂O₂ synthesis, Photo-redox center, Spatial separation, Synergistic utilization, Polymer photocatalyst

Yao Xie, Qitao Zhang, Hongli Sun, Zhenyuan Teng, Chenliang Su. Semiconducting Polymers for Photosynthesis of H₂O₂: Spatial Separation and Synergistic Utilization of Photoredox Centers[J]. Acta Phys. -Chim. Sin. 2023, 39(11), 2301001. doi: 10.3866/PKU.WHXB202301001

Figures/Tables 18

References 88

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Reaction conditions	Photocatalysts	Yield of H₂O₂	Ref.
Sacrificial agent	MIL-125-R7	2.4 mmol·L⁻¹/3 h	68
	TA-Por-sp²-COF	28.3 mmol·L⁻¹/2 h	53
	CKCN-0.03	1.908 mmol·L⁻¹/h	12
	3DBC-C₃N₄-N	3.3 mmol·L⁻¹/h	60
	Ni-CAT-CN₆₀	1.2 mmol·L⁻¹/h	61
	Ar-C₃N₄	1.22 mmol·L⁻¹/h	22
	O-CNC	2.01 mmol·L⁻¹/h	62
	TF50-COF	0.174 mmol·L⁻¹/h	28
	Nv—C≡N—CN	3.093 mmol·L⁻¹/h	63
Pure water (4e⁻ WOR)	TPE-AQ	0.455 mmol·L⁻¹/h	31
	TPB-DMTP-COF	≈ 0.58 mmol·L⁻¹/h	27
	RF523	≈ 5.4 mmol·L⁻¹/5 h	33
	RF/P3HT-1.0	≈ 2.31 mmol·L⁻¹/5 h	34
	MRFS-7	≈ 0.284 mmol·L⁻¹/h	35
	MRF-250	0.97 mmol·L⁻¹/h	37
	PCNBA0.2	≈ 0.069 mmol·L⁻¹/h	59
	Sb-SAPC15	0.365 mmol·L⁻¹/2h	43
	g-C₃N₄/PDI/rGO_0.05	≈ 1.238 mmol·L⁻¹/2h	64
	PM-CDs-30	0.268 mmol·L⁻¹/h	65
	Nv—C≡N—CN	0.137 mmol·L⁻¹/h	63
Pure water (2e⁻ WOR)	CTF-EDDBN	≈ 0.033 mmol·L⁻¹/h	38
	CTF-BDDBN	≈ 0.068 mmol·L⁻¹/h	38
	CHF-DPA	≈ 2.75 mmol·L⁻¹/h	32
	CHF-DPDA	≈ 3.46 mmol·L⁻¹/h	32
	COF-TfpBpy	1.042 mmol·L⁻¹/h	66

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Semiconducting Polymers for Photosynthesis of H₂O₂: Spatial Separation and Synergistic Utilization of Photoredox Centers

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	Reaction modes	Typical photocatalysts	Reduction center products	Oxidation center products	Ref.
Type Ⅰ		MIL-125-Rn	H₂O₂	Benzaldehyde	68
		TA-Por-sp²-COF	H₂O₂	N-Benzylidenebenzylamine	53
		PFBTPCBM	H₂O₂	Formate	69
Type Ⅱ		PCN-10-CP-10	H₂	H₂O₂	73
		C-N-g-C₃N₄	H₂	H₂O₂	74
		CoP/CDs	H₂O₂ & H₂	O₂	75
		24%-WO₃-MIL-100-Fe	CH₄ & CO	H₂O₂	76
Type Ⅲ-4e⁻ WOR		Nv—C≡N—CN	H₂O₂	O₂	63
		g-C₃N₄/PDI/rGO_0.05	H₂O₂	O₂	64
		MRFS-7	H₂O₂	O₂	35
		TPE-AQ	H₂O₂	O₂	31
		Sb-SAPC15	H₂O₂	O₂	43
Type Ⅲ-2e− WOR		CTF-EDDBN	H₂O₂	H₂O₂	38
		CTF-BDDBN	H₂O₂	H₂O₂	38
		COF-TfpBpy	H₂O₂	H₂O₂	66

Semiconducting Polymers for Photosynthesis of H2O2: Spatial Separation and Synergistic Utilization of Photoredox Centers

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Semiconducting Polymers for Photosynthesis of H₂O₂: Spatial Separation and Synergistic Utilization of Photoredox Centers