低铱酸性氧析出电催化剂的研究进展

doi:10.13208/j.electrochem.2214010

电化学（中英文） ›› 2022, Vol. 28 ›› Issue (9): 2214010. doi: 10.13208/j.electrochem.2214010

所属专题： “电催化和燃料电池”专题文章

低铱酸性氧析出电催化剂的研究进展

倪静¹^,², 施兆平¹^,², 王显¹^,², 王意波¹^,², 吴鸿翔¹^,², 刘长鹏¹^,²^,^*(), 葛君杰¹^,²^,³^,^*(), 邢巍¹^,²^,^*()

1.中国科学院长春应用化学研究所,吉林省先进低碳化学电源重点实验室,电分析化学国家重点实验室,吉林长春 130022
2.中国科学技术大学应用化学与工程学院,安徽合肥,230026
3.中国科学院大连洁净能源创新研究院,辽宁大连116023

收稿日期:2022-07-08 修回日期:2022-07-21 出版日期:2022-09-28 发布日期:2022-08-17
通讯作者: 刘长鹏,葛君杰,邢巍 E-mail:liuchp@ciac.ac.cn;gejj@ciac.ac.cn;xingwei@ciac.ac.cn

Recent Development of Low Iridium Electrocatalysts toward Efficient Water Oxidation

Jing Ni¹^,², Zhao-Ping Shi¹^,², Xian Wang¹^,², Yi-Bo Wang¹^,², Hong-Xiang Wu¹^,², Chang-Peng Liu¹^,²^,^*(), Jun-Jie Ge¹^,²^,³^,^*(), Wei Xing¹^,²^,^*()

1. State Key Laboratory of Electroanalytic Chemistry, Jilin Province Key Laboratory of Low Carbon Chemistry Power, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences,Changchun 130022, China
2. School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China
3. Dalian National Laboratory for Clean Energy,Chinese Academy of Sciences, Dalian 116023, China

Received:2022-07-08 Revised:2022-07-21 Published:2022-09-28 Online:2022-08-17
Contact: Chang-Peng Liu,Jun-Jie Ge,Wei Xing E-mail:liuchp@ciac.ac.cn;gejj@ciac.ac.cn;xingwei@ciac.ac.cn
About author:First author contact:
#These authors contributed equally to this work.

摘要/Abstract

摘要：

开发高性能、低成本的氧析出反应（OER）电催化剂是促进质子交换膜水电解（PEMWE）制氢规模化应用的关键。迄今为止, OER催化剂的最佳选项仍为贵金属铱(Ir), 但其仍存在活性不足和储量稀缺的问题, 进而增加了材料成本和电力成本。因此, 开发低Ir载量、高活性和稳定性间距, 且能够满足PEMWE设备中大电流密度和长期运行要求的OER催化剂是十分必要的。这些目标的实现需要深入理解酸性OER机制、明晰材料设计方法, 并建立可靠的性能评估指标（特别是对耐久性的评估）。综上,本文首先系统总结了目前被广泛接受的酸性OER活性表达机制（即吸附析出机制、晶格氧氧化机制和多活性中心机制）和失活机制（即活性物种溶解、晶相和形态演化、催化剂脱落和活性位点阻塞）, 为催化剂的微观结构设计提供指导。其次, 我们讨论了最近报道的几类低铱OER催化剂, 包括多金属合金氧化物、负载型催化剂、具有特殊空间结构的催化剂和单位点催化剂, 并重点描述低Ir催化剂中的性能如何得以调控以及其中潜在的构效关系。随后, 我们介绍了常用的催化剂稳定性评价指标、催化剂失活表征技术以及模拟PEMWE实际操作条件的催化剂寿命测试方法,希望为催化剂筛选提供依据。最后, 针对未来可用于PEMWE体系的低铱OER催化剂的探索提出了一些可行建议。

关键词: 氧析出反应, 质子交换膜水电解, 低铱载量, 活性稳定性机制, 稳定性评估指标

Abstract:

Developing high-performance and low-cost electrocatalysts for oxygen evolution reaction (OER) is the key to implementing polymer electrolyte membrane water electrolyzer (PEMWE) for hydrogen production. To date, iridium (Ir) is the state-of-the-art OER catalyst, but still suffers from the insufficient activity and scarce earth abundance, which results in high cost both in stack and electricity. Design low-Ir catalysts with enhanced activity and stability that can match the requirements of high current and long-term operation in PEMWE is thus highly desired, which necessitate a deep understanding of acidic OER mechanisms, unique insights of material design strategies, and reliable performance evaluation norm, especially for durability. With these demand in mind, we in this review firstly performed a systematic summary on the currently recognized acidic OER mechanism on both activity expression (i.e. the adsorbate evolution mechanism, the lattice oxygen mediated mechanism and the multi-active center mechanism) and inactivation (i.e. active species dissolution, evolution of crystal phase and morphology, as well as catalyst shedding and active site blocking), which can provide guidance for material structural engineering towards higher performance in PEMWE devices. Subsequently, we critically reviewed several types of low-Ir OER catalysts recently reported, i.e. multimetallic alloy oxide, supported, spatially structured and single site catalysts, focusing on how the performance has been regulated and the underlying structure-performance relationship. Lastly, the commonly used indicators for catalyst stability evaluation, wide accepted deactivation characterization techniques and the lifetime probing methods mimicking the practical operation condition of PEMWE are introduced, hoping to provide a basis for catalyst screening. In the end, few suggestions on exploring future low-Ir OER catalysts that can be applied in the PEMWE system are proposed.

Key words: oxygen evolution reaction, polymer electrolyte membrane water electrolysis, low-iridium, catalytic mechanism on activity and stability, evaluation criteria for operational stability

倪静, 施兆平, 王显, 王意波, 吴鸿翔, 刘长鹏, 葛君杰, 邢巍. 低铱酸性氧析出电催化剂的研究进展[J]. 电化学（中英文）, 2022, 28(9): 2214010.

Jing Ni, Zhao-Ping Shi, Xian Wang, Yi-Bo Wang, Hong-Xiang Wu, Chang-Peng Liu, Jun-Jie Ge, Wei Xing. Recent Development of Low Iridium Electrocatalysts toward Efficient Water Oxidation[J]. Journal of Electrochemistry, 2022, 28(9): 2214010.

图/表 16

Catalyst	Electrode	Electrolyte solution	Concentration	Ir loading/ μg·cm^-2	Overpoten- tial@ 10 mA·cm^-2/ mV	Cell voltage@ 1 A·cm^-2/V	Stability	Ref.
Ir-Ni(9.3)	Gold working electrode	HClO₄	0.1 mol·L^-1	30.6	~ 270			[45]
Ir-Ni(9.3)	Nafion			100		~1.60		[45]
Cu_0.5Ir_0.5O_δ	Ti plate	HClO₄	0.1 mol·L^-1	~200	~368			[46]
IrCoNi PHNC	GC	HClO₄	0.1 mol·L^-1	10	303		1 h@5 mA·cm^-2	[47]
9R-BaIrO₃	GC	H₂SO₄	0.5 mol·L^-1	~178	230		48 h@10 mA·cm^-2	[48]
Au@AuIr₂	GC	H₂SO₄	0.5 mol·L^-1	20	261		30 h@10 mA·cm^-2	[49]
IrHf_xO_y	Au	HClO₄	0.1 mol·L^-1	~ 0.6	~ 330		6 h@5 mA·cm^-2	[50]
Gd-pIrO₂	GC	H₂SO₄	0.5 mol·L^-1	278	287		6 h@10 mA·cm^-2	[51]
Ir-MoO₃	CP	H₂SO₄	0.5 mol·L^-1	~ 77	156		50 h@10 mA·cm^-2	[52]
Ir@WO_xNR	W foil	H₂SO₄	0.5 mol·L^-1	144	330		10 h@100 mA·cm^-2	[53]
Ir@WO_xNR	Nafion115			144		1.79	1030 h@0.5 A·cm^-2	[53]
IrO₂@Ir/TiN	GC	H₂SO₄	0.5 mol·L^-1	379	265		6 h@10 mA·cm^-2	[54]
IrO₂@α-MnO₂	Ti plate	HClO₄	0.1 mol·L^-1	200	275		5 h@10 mA·cm^-2	[55]
Ir-Pt-TiO₂	Au	HClO₄	0.1 mol·L^-1	3.49	> 570		5 h@1.8 V	[56]
Ir-Pt-TiO₂	Nafion117			1000		~ 1.90		[56]
IrO_x/ATO	GC	H₂SO₄	0.05 mol·L^-1	10.2	~ 430		15 h@1 mA·cm^-2	[57]
IrO_x/ATO	Nafion212			1000		~ 1.69		[57]
Ir/Fe₄N	GC	H₂SO₄	0.5 mol·L^-1	76.5	316		2 h@10 mA·cm^-2	[58]
IrO₂(1:100)- 450 ^°C	GC	H₂SO₄	0.5 mol·L^-1	324	282		2 h@1.56 V	[59]
IrO₂(1:100)- 450 ^°C	Nafion117			1714		1.649		[59]
IrO₂ NN-L	GC	H₂SO₄	1 mol·L^-1	214	313		2 h@10 mA·cm^-2	[60]
IrO₂ NN-L	Nafion117			3428		~ 1.80	250 h@2 A·cm^-2	[60]
Ir NF	GC	H₂SO₄	0.05 mol·L^-1	200	430			[6]
Ir NF	Nafion115			200		~ 1.75		[6]
Ir NSs	GC	H₂SO₄	0.5 mol·L^-1	137	240		8 h @10 mA·cm^-2	[61]
1T-IrO₂	GC	HClO₄	0.1 mol·L^-1	177	197		45 h@50 mA·cm^-2	[62]
1T-IrO₂	Nafion117			850		1.5 V@ 253 mA cm^-2	126@250 mA·cm^-2	[62]
3R-IrO₂	GC	HClO₄	0.1 mol·L^-1	~231	188		511 h@10 mA·cm^-2	[63]
Ir_0.06Co_2.94O₄	Au	HClO₄	0.1 mol·L^-1	~5.2	292		200 h @10 mA·cm^-2	[64]
Ir-MnO₂	CP	H₂SO₄	0.5 mol·L^-1	192	218		650 h@10 mA·cm^-2	[65]
Ir-NiCo₂O₄ NSs	CC	H₂SO₄	0.5 mol·L^-1	2.44	240		70 h@10 mA·cm^-2	[66]
AD-HN-Ir	CP	H₂SO₄	0.5 mol·L^-1	3.5	216		100 h@10 mA·cm^-2	[67]

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Mechanism	AEM	LOM	OPM
Catalytic process	Cation redox	Anion redox	Cation redox
Theoretical overpotential	Limited by the scaling relation between OH* and OOH*, minimum value of ~ 0.37 V	Minimum value of ~0.17 V	No related reports
Active site	Single coordination unsaturated metal sites	Single coordination unsaturated oxygen sites	Two coordinations unsaturated metal sites with suitable distance
Identification method	In situ attenuated total reflection infrared	Isotope labelled in situ differential electrochemical mass spectra	Operando synchrotron FT infrared

低铱酸性氧析出电催化剂的研究进展

Recent Development of Low Iridium Electrocatalysts toward Efficient Water Oxidation

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