过渡金属氧化物/硫属化合物用于电化学氧还原制过氧化氢

doi:10.3866/PKU.WHXB202407005

物理化学学报 >> 2024, Vol. 40 >> Issue (12): 2407005.doi: 10.3866/PKU.WHXB202407005

所属专题：太阳燃料制备

过渡金属氧化物/硫属化合物用于电化学氧还原制过氧化氢

朱潇锋¹^,²^,†^,*(), 肖兵兵¹^,²^,†, 苏家欣¹^,², 王帅³, 张清然³^,*(), 王骏¹^,²^,*()

¹ 西南科技大学材料与化学学院, 环境友好能源材料国家重点实验室, 绵阳 621010
² 西南科技大学成都创新研究院, 成都 610299
³ 同济大学环境科学与工程学院, 上海污染控制与生态安全研究院, 污染控制与资源化研究国家重点实验室, 上海 200092

收稿日期:2024-07-07 修回日期:2024-08-03 录用日期:2024-08-03 发布日期:2024-11-09
通讯作者: Email: junwang091@163.com (王骏)xfzhu@swust.edu.cn (朱潇锋)qingran_zhang@tongji.edu.cn (张清然)
作者简介:
^†These authors contributed equally to this work.
基金资助:
国家自然科学基金(52202305); 国家自然科学基金(22176155); 四川省自然科学基金(2023NSFSC0095); 四川省杰出青年项目(22JCQN0061); 西南科技大学龙山人才引进计划(22zx7103); 四川省留学回国人员科技活动项目择优资助项目(22zd3148)

Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides

Xiaofeng Zhu¹^,²^,*(), Bingbing Xiao¹^,², Jiaxin Su¹^,², Shuai Wang³, Qingran Zhang³^,*(), Jun Wang¹^,²^,*()

¹ State Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang 621010, Sichuan Province, China
² Tianfu Institute of Research and Innovation, Southwest University of Science and Technology, Chengdu 610299, China
³ State Key Laboratory of Pollution Control and Resources Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, Shanghai 200092, China

Received:2024-07-07 Revised:2024-08-03 Accepted:2024-08-03 Published:2024-11-09
Contact: Email: junwang091@163.com (Jun Wang)xfzhu@swust.edu.cn (Xiaofeng Zhu)qingran_zhang@tongji.edu.cn (Qingran Zhang)
Supported by:
the National Natural Science Foundation of China(52202305); the National Natural Science Foundation of China(22176155); National Natural Science Foundation of Sichuan Province, China(2023NSFSC0095); Outstanding Youth Talents of Sichuan Science and Technology Program(22JCQN0061); Long Shan Talents Plan of SWUST(22zx7103); Scientific Research Foundation for the Returned Overseas Chinese Scholars, Department of Human Resource and Social Security of Sichuan Province(22zd3148)

摘要/Abstract

摘要：

利用两电子路径的电化学氧还原反应来合成过氧化氢已成为一种极具潜力和低碳新型化工技术。过去的研究和成果主要致力于开发新型的碳基电催化剂。然而，碳基催化材料的合成过程复杂、高电位选择性不稳定且活性位点不明确等问题一直被广泛诟病。基于此，催化稳定性较高且材料微结构调控性较好的过渡金属氧化物和硫属化合物在两电子氧还原上的应用开始加速涌现。因此，本综述对此类材料用于氧气-过氧化氢电化学转换的金属氧化物和硫属化合物发展进行前瞻性讨论。首先，针对其多样性和催化活性，从实验合成和理论模拟的角度进行综述。同时，根据其形貌、相组成、掺杂和缺陷调控，对氧化物和硫属化合物的拓扑结构和化学特性与两电子选择性的潜在关系进行剖析。进而，对金属氧化物和硫属化合物的活性位点和反应机理等相关研究进展进行了讨论和总结。最后，对过渡金属氧化物和硫属化合物在两电子氧还原制取过氧化氢上的应用挑战和前景进行了分析，并提出了相关的建议。本综述提供了金属氧化物/硫属化合物在两电子氧还原上的基础研究及分析，以推动其在能源相关产业上的实际应用。

关键词: 氧化物, 硫属化合物, 氧还原反应, 过氧化氢电合成, 活性位点

Abstract:

Electrochemical oxygen reduction reaction via the two-electron pathway (2e-ORR) is becoming a promising and sustainable approach to producing hydrogen peroxide (H₂O₂) without significant carbon footprints. To achieve better performance, most of the recent progress and investigations have focused on developing novel carbon-based electrocatalysts. Nevertheless, the sophisticated preparations, decreased selectivity and undefined active sites of carbon-based catalysts have been generally acknowledged and criticized. To this end, transition metal oxides and chalcogenides have increasingly emerged for 2e-ORR, due to their catalytic stability and tunable microstructure. Here, the development of metal oxides and chalcogenides for O₂-to-H₂O₂ conversion is prospectively reviewed. By summarizing previous theoretical and experimental efforts, their diversity and outstanding catalytic activity are firstly provided. Meanwhile, the topological and chemical factors influencing 2e-ORR selectivity of the metal oxides/chalcogenides are systematically elucidated, including morphology, phase structures, doping and defects engineering. Thus, emphasizing the influence on the binding of ORR intermediates, the active sites and the underlying mechanism is highlighted. Finally, future opportunities and challenges in designing metal oxides/chalcogenides-based catalysts for H₂O₂ electro-synthesis are outlined. The present review provides insights and fundamentals of metal oxides/chalcogenides as 2e-ORR catalysts, promoting their practical application in the energy-related industry.

Key words: Oxides, Chalcogenides, Oxygen reduction reaction, H₂O₂ electro-synthesis, Active sites

朱潇锋, 肖兵兵, 苏家欣, 王帅, 张清然, 王骏. 过渡金属氧化物/硫属化合物用于电化学氧还原制过氧化氢[J]. 物理化学学报, 2024, 40(12), 2407005. doi: 10.3866/PKU.WHXB202407005

Xiaofeng Zhu, Bingbing Xiao, Jiaxin Su, Shuai Wang, Qingran Zhang, Jun Wang. Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides[J]. Acta Phys. -Chim. Sin. 2024, 40(12), 2407005. doi: 10.3866/PKU.WHXB202407005

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202407005

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I12/2407005

图/表 11

表1

表2

图1

表3

Type	Catalyst	Electrolytes	2e-ORR Performance	Ref.
Metal oxides	NiO_x-C	0.1 M KOH	Onset: 0.76 V_RHE	53
			Selectivity: 91%
	Co₃O₄	0.5 M H₂SO₄	Selectivity: 60%	54
			Yield: 1.6 mol∙g_cat⁻¹∙h⁻¹ at 0.0 V_RHE
			Stability: 5 h at 0.1 V_RHE
	In₂O₃/CDs	0.1 M KOH	Selectivity: nearly 100%	55
			Yield: 4.5 mol∙g_cat⁻¹∙h⁻¹
			Stability: 5, 000 ADT cycles at 0.5 V_RHE
	MnO₂/C	H₂SO₄ 0.1 M + K₂SO₄ 0.1 M	Yield: 391 mg∙L⁻¹	56
	ZnO/rGO	0.5 M NaCl	Selectivity: 80%	57
	ZnCo₂O₄/g-C₃N₄	0.1 M KOH	Selectivity: 86.74%	58
	ZnO/ZnS@C	0.1 M KOH	Selectivity: 90%	60
			Yield: 16 mmol∙g_cat⁻¹∙h⁻¹
			Stability: 30 h at 0 V_RHE
	V₂O₅-Ov	0.1 M KOH	Selectivity: 92.32%	61
			Yield: 1.96 mol∙g_cat⁻¹∙h⁻¹
			FE: 84%
	Nd-doped Bi₄Ti₃O₁₂	0.1 M KOH	Selectivity: 95%	62
			Yield: 208 mmol∙g_cat⁻¹∙h⁻¹ at 0.36 V_RHE
			FE: 97.6%
Metal oxides	NiNb₂O₆	0.1 M KOH	Selectivity: 96%	63
			Yield: 996 mmol∙g_cat⁻¹∙h⁻¹
			FE: 92%
			Stability: 24 h at 0.3 V_RHE
	Pr₂Ni_0.8Mo_0.2O_4+δ	0.1 M KOH	Selectivity: 79%	64
			Stability: 24 h at 10 mA∙cm⁻²
	Pb-(NiWMnNbZrTi)_1/6O₃	0.1 M KOH	Selectivity: 91%	66
			Stability: 12 h at 0.1 V_RHE
	CoAl₂O₄/CoO	0.1 M KOH	Selectivity: 85%	67
			Yield: 1.446 mol∙g_cat⁻¹∙h⁻¹
			Stability: 7 h at 0.2 V_RHE
	ZrO₂/PL₆C	0.1 M K₂SO₄	Selectivity: 88.8%	68
	α-Fe₂O₃	0.1 M KOH 0.1 M Na₂SO₄	Selectivity: 90%, 88%, and 95% in acidic, neutral, and alkaline electrolytes	69
		5 mM H₂SO₄	Yield: 454 mmol∙g_cat⁻¹∙h⁻¹ at 0.1 V_RHE in alkaline
			FE: 80.5% in AEM-flow cell
			Stability: 48 h at 0.5 V_RHE
	c-WO₃	0.1 M KOH	Selectivity: 90%	110
			Yield: 179 mmol∙g_cat⁻¹∙h⁻¹
			Stability: 24 h at 0.1 V_RHE
	Fe-CeO₂	0.1 M KOH	Selectivity: 97.7% at 0.38 V_RHE	112
			Yield: 1.80 mol∙g_cat⁻¹∙h⁻¹ at 0.1 V_RHE
			FE: 94% at 0.1 V_RHE
			Stability: 10 h at 0.5 V_RHE
	Mn-TiO₂	0.1 M KOH	Onset: 0.78 V_RHE	113
			Selectivity: 92.7%
			Yield: 205 mg∙L⁻¹ h⁻¹ at 0 V_RHE
			FE: 98% at 0.3 V_RHE
			Stability: 12 h at 0.40 V_RHE
Metal chalcogenides	L-PdS-Vs metallene	0.1 M KOH	Selectivity: 90%	70
			Yield: 1.12 mol∙g_cat⁻¹∙h⁻¹ at 0.3 V_RHE
			FE: 90%
			Stability: 5, 000 CV cycles
	Pd-S NCs	0.05 M H₂SO₄	Selectivity: 90%	71
			Yield: 12.5 mM at 0.2 V_RHE
	CuNW@CoS₄	0.1 M Na₂SO₄ pH = 5	Selectivity: 93%	72
			FE: 91% at 0.1 V_RHE
			Stability: 5 h at 0.1 V_RHE
	CoSe₂ polymorph	0.05 M H₂SO₄	Yield: 547 mg∙L⁻¹	74
	NiS₂ nanosheets	0.05 M H₂SO₄	Selectivity: 99%, onset ~130 mV	75
			Yield: 109 mg∙L⁻¹∙h⁻¹ 0.156 V_RHE
			FE: 98% at 0.456 V_RHE
	Mn-CuS-2	0.1 M KOH	Selectivity: 92%	76
			Yield: 90 mmol∙g_cat⁻¹∙h⁻¹
			Stability: 25 h at 0.6 V_RHE
	Cu-defective Au@Cu_2-xS-CNTs	0.1 M KOH	Selectivity: 94%	77
			Stability: 10 h at 0.5 V_RHE
Metal chalcogenides	Ti-ZnCoS HSS	0.1 M KOH	Selectivity: 98%	78
			Yield: 675 mmol∙g_cat⁻¹∙h⁻¹
			Stability: 12 h at 0.55 V_RHE
	Ni₂Mo₆S₈	0.1 M KOH	Selectivity: 90%	79
			Yield: 90 mmol∙g_cat⁻¹∙h⁻¹
			Stability: 10 h at 0.5 V_RHE
Metal chalcogenides	CuCo_0.8Ni_1.2S₄	0.05 M H₂SO₄	Selectivity: 60%	80
	Pd-Se-B NC	0.1 M KPi buffer	Selectivity: 85%	81
	PtSe₂/C	0.1 M HClO₄	Selectivity: 91%	82
	Pd₄Se NPs	0.1 M HClO₄ 0.1 M KCl	Selectivity: 93.5%, 89.7%, and 86.7% in acidic, neutral, and alkaline electrolytes	83
		0.1 M KOH
	a-PdSe₂ NPs	0.1 M KOH	Selectivity: 90% in different electrolytes⁻¹∙h⁻¹	84
		0.1 M HClO₄ 0.1 M Na₂SO₄	Yield: 3245.7, 1725.5, and 2242.1 mmol∙g_Pd in alkaline, acidic, and neutral electrolytes
	Cu_7.2Se₄	0.1 M KOH	Selectivity: 90%	85
	Fe-CoSe-HT	0.1 M KOH 0.1 M Na₂SO₄	Selectivity: 99.1%, 83.2% and 93.6% in alkaline, neutral, and acidic electrolytes	86
		0.05 M H₂SO₄	Stability: 18 h at 0.2 V_RHE
	sc-CoSe₂	0.5 M H₂SO₄	FE: 96.7%	88
			Yield: 30.60 mg∙cm⁻²∙h⁻¹
			Stability: 100 h at 63 mA∙cm⁻²
	CoPSe	0.1 M HClO₄	Selectivity: 76%-85% in 0–0.5 V_RHE	89
			Stability: 10 h at 0.1 V_RHE
	CoSe₂@NCNTs	0.1 M HClO₄	Selectivity: 93.2%	90
			Yield: 172 mg∙L⁻¹∙h⁻¹
			Stability: 24 h at 0.1 V_RHE
	CoSe₂ NS/CC	0.1 M KOH	Selectivity: 92%	96
			Stability: 10 h at 0.5 V_RHE
	NiSe₂-V_Se	0.1 M KOH	Selectivity: 96%	97
			Stability: 40, 000 s at 0.4 V_RHE
	NiSe₂/CP	0.05 M H₂SO₄	Selectivity: 92%	99
			Yield: 988 mg∙L⁻¹
			Stability: 12 h at 0 V_RHE
	Pd-Te	0.1 M H₂SO₄	Selectivity: 75%	101
	CoTe@NC	0.1 M HClO₄	Selectivity: 92.6%	103
			Yield: 297.9 mg∙L⁻¹∙h⁻¹
			Stability: 12 h at 0.4 V_RHE
	2H-MoTe₂ nanoflakes	0.5 M H₂SO₄	Onset: 140 mV	104
			Selectivity: 93%

表3

图2

图3

图4

图5

图6

图7

图8

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ORR pathway	Reaction equations and standard potentials
ORR pathway	Alkaline electrolytes	Acidic electrolytes
4e-ORR	O₂ + 2H₂O + 4e^- → 4OH^- (E⁰ = 1.23 V)	O₂ + 4H⁺ + 4e^- → 2H₂O (E⁰ = 1.23 V)
2e-ORR	O₂ + H₂O + 2e^- → HO₂^- + OH^- (E⁰ = 0.76 V)	O₂ + 2H⁺ + 2e^- → H₂O₂ (E⁰ = 0.70 V)
(2e + 2e)-ORR	HO₂^- + H₂O + 2e^- → 3OH^- (E0 = 0.86 V)	H₂O₂ + 2H⁺ + 2e^- → 2H₂O (E⁰ = 1.76 V)

In alkaline electrolytes	In acidic electrolytes
O₂ + H₂O + e⁻ + * → *OOH + OH⁻	O₂ + H⁺ + e⁻ + * → *OOH
OOH + e⁻→ HO₂⁻ +	OOH + H⁺ + e⁻ → + H₂O₂

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过渡金属氧化物/硫属化合物用于电化学氧还原制过氧化氢

Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides

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