电催化氯代芳香烃脱氯催化剂的合成策略、应用与挑战

doi:10.1016/j.actphy.2025.100120

物理化学学报 >> 2025, Vol. 41 >> Issue (10): 100120.doi: 10.1016/j.actphy.2025.100120

电催化氯代芳香烃脱氯催化剂的合成策略、应用与挑战

王琪¹^,², 刘宇庆¹, 王洁菲¹, 马媛媛¹^,*(), 都京¹^,*(), 韩占刚¹^,*()

¹ 河北师范大学化学与材料科学学院, 分析测试中心, 国家级实验化学教育示范中心, 河北薄膜太阳能电池材料与器件工程研究中心, 河北能源转换材料与器件技术创新中心, 河北石家庄 050024
² 邢台学院化学工程与生物技术学院, 河北邢台 054001

收稿日期:2025-04-16 修回日期:2025-05-25 录用日期:2025-06-11 发布日期:2025-09-29
通讯作者: Email: mayy334@hebtu.edu.cn (马媛媛)duj622@hebtu.edu.cn (都京)hanzg116@hebtu.edu.cn (韩占刚)
基金资助:
国家自然科学基金(22471056); 国家自然科学基金(22301058); 国家自然科学基金(22371065); 河北省自然科学基金(B2024205033); 河北省自然科学基金(B2024205007); 河北省自然科学基金(B2022205005); 河北省教育厅科学技术研究项目(QN2023049); 中国博士后科学基金资助项目(2021TQ0095); 河北省科技厅项目(22567622H); 河北师范大学科研基金(L2023B51); 河北师范大学化学博士后科研流动站

Catalysts for electrocatalytic dechlorination of chlorinated aromatic hydrocarbons: synthetic strategies, applications, and challenges

Qi Wang¹^,², Yuqing Liu¹, Jiefei Wang¹, Yuan-Yuan Ma¹^,*(), Jing Du¹^,*(), Zhan-Gang Han¹^,*()

¹ Hebei Technology Innovation Center for Energy Conversion Materials and Devices, Hebei Engineering Research Center of Thin Film Solar Cell Materials and Devices, National Demonstration Center for Experimental Chemistry Education, Testing and Analysis Center, College of Chemistry and Materials Science, Hebei Normal University, Shijiazhuang 050024, Hebei Province, China
² College of Chemistry and Chemical Engineering, Xingtai University, Xingtai 054001, Hebei Province, China

Received:2025-04-16 Revised:2025-05-25 Accepted:2025-06-11 Published:2025-09-29
Contact: Email: mayy334@hebtu.edu.cn (Yuan-Yuan Ma)duj622@hebtu.edu.cn (Jing Du)hanzg116@hebtu.edu.cn (Zhan-Gang Han)
Supported by:
the National Natural Science Foundation of China(22471056); the National Natural Science Foundation of China(22301058); the National Natural Science Foundation of China(22371065); the Natural Science Foundation of Hebei Province(B2024205033); the Natural Science Foundation of Hebei Province(B2024205007); the Natural Science Foundation of Hebei Province(B2022205005); the Science and Technology Project of Hebei Education Department(QN2023049); the China Postdoctoral Science Foundation funded project(2021TQ0095); the Project of Science and Technology Department of Hebei Province(22567622H); the Science Foundation of Hebei Normal University(L2023B51); the Chemistry Postdoctoral Research Station at Hebei Normal University

摘要/Abstract

摘要：

电催化脱氯(EHDC)因其高效率、无二次污染及反应条件温和等特点，被认为是极具前景的污染物降解技术。在EHDC过程中，活性氢的生成、C―Cl键的断裂以及氯代芳香烃或反应中间体的吸附/脱附是核心步骤。该技术依赖高活性电催化剂以提升催化效率与成本效益。本文首先系统总结了EHDC中催化剂活性与稳定性的评价方法和指标，分别从贵金属与非贵金属基催化剂体系出发，综述了近年来低成本、高性能电催化剂的前沿进展。重点探讨了催化剂构效关系及提高催化剂活性的关键策略，如构建异质界面和设计合金结构优化活性组分的电子结构特性以及调控催化剂局域微环境改善电荷转移效率等。此外，还探讨了氯代芳香烃的结构对电催化脱氯活性的影响关系。最后分析了当前电催化加氢脱氯技术面临的挑战与未来发展方向，为含氯有机物的高效脱氯转化研究提供理论和技术参考。

关键词: 电催化脱氯, 含氯有机物, 电催化剂, 构筑策略

Abstract:

Electrocatalytic hydrodechlorination (EHDC) is a promising technology for degrading chlorinated aromatic hydrocarbons (CAHs), offering high efficiency, minimal secondary pollution, and mild operating conditions. Its effectiveness relies on three critical steps: atomic hydrogen (H*) generation, C―Cl bond cleavage, and adsorption/desorption of CAHs/products. Developing high-performance electrocatalysts is essential to optimize energy efficiency and cost-effectiveness. It is urgent to summarize research progress on design strategies for catalysts and establish fundamental principles. In this review, we first summarize commonly deployed measurement methods and metrics for assessing catalyst activity and stability in EHDC. Then, a series of strategies for enhancing the production of H*, facilitating the cleavage of C―Cl bonds, and optimizing the adsorption and desorption kinetics of CAHs and their intermediates/products on the catalyst surface are summarized. These strategies include the loading of catalysts on carbon-based/transition-based support to enhance the dispersion of Pd; constructing heterostructures or forming alloys to modulate the electronic structure of active metal nanocatalysts and optimize its binding affinities with reactants and intermediates; and modulating the microenvironment to modify the interface hydrophilicity/hydrophobicity of catalyst to increase reaction rates or improve stability of catalysts. Additionally, the applications of electrocatalysts for EHDC in recent years, such as Pd-based supported electrocatalysts, Pd-based heterostructure electrocatalysts, Pd-based alloy electrocatalysts, and noble-metal-free electrocatalysts are discussed, as well as the influence of catalyst composition on performance. It is noted that the EHDC efficiency of CAHs is influenced not only by the catalyst but also significantly correlated with the structure of CAHs. Thus, the effects of CAHs structures on EHDC performance are also discussed. Studies demonstrate that weak adsorption between the electrode and CAHs is more conducive to EHDC reactions. The number and position of chlorine functional groups, steric hindrance, and the properties of other functional groups in the substrate molecule can also influence EHDC performance. Finally, the challenges and future prospects of EHDC are highlighted, including improving the catalytic performance of non-noble catalysts, employing advanced in situ and operando characterization techniques, and optimizing DFT calculations to more closely align with real catalytic conditions, all aiming to inspire new investigations and advancements in the field of EHDC of CAHs.

Key words: Electrocatalytic hydrodechlorination, Chlorinated aromatic hydrocarbon, Electrocatalyst, Construction strategy

王琪, 刘宇庆, 王洁菲, 马媛媛, 都京, 韩占刚. 电催化氯代芳香烃脱氯催化剂的合成策略、应用与挑战[J]. 物理化学学报, 2025, 41(10), 100120. doi: 10.1016/j.actphy.2025.100120

Qi Wang, Yuqing Liu, Jiefei Wang, Yuan-Yuan Ma, Jing Du, Zhan-Gang Han. Catalysts for electrocatalytic dechlorination of chlorinated aromatic hydrocarbons: synthetic strategies, applications, and challenges[J]. Acta Phys. -Chim. Sin. 2025, 41(10), 100120. doi: 10.1016/j.actphy.2025.100120

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100120

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I10/100120

图/表 34

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表1

Catalyst	CAHs	EHDC efficiency	k_ap (min⁻¹)	Mass Activity	CE (%)	TOF (h⁻¹)	Reference
C-Pd	2, 4-DCP	91.44%	0.118	–	–	–	[28]
C-Pd	2, 4-DCP	66.4%	–	–	35	–	[4]
Pd/MWCNTs-B	4-CP	100%	0.0971	–	54	–	[51]
Pd/MWCNTs-E	4-CP	60%	–	–	–	–	[51]
Pd/MWCNTs-H	4-CP	29%	–	–	–	–	[51]
Pd/PCN-08	4-CP	85%	0.039	–	17.7	22.8	[30]
P-Pd@MX–CC	DCF	94.6 ± 0.1%	0.39	–	–	–	[52]
Pd/Ni foam electrode	4-MCB	94.6%	0.11	–	24.6	–	[5]
Pd/foam-Ni	4-CP	100%	0.04733	–	24	–	[60]
Pd-NiMOF–Ni	2, 4-D	99.8%	–	–	–	–	[64]
Pd-NiRu-MOF–NF	2-CP	100%	0.0731	–	14.2	–	[65]
Pd@CoFe_V-LDH–NF	2, 4-DCP	95.46%	0.023	–	–	–	[44]
Pd/Ni_xAl_100−x-LDH-OH_V)	2, 4-DCP	–	–	6.54 min⁻¹·g⁻¹	10.6	–	[50]
NiFeP-Pd stems	4-CP	98.8%	0.044	446.01 min⁻¹·g⁻¹	16	–	[45]
Pd/Ni-Cu-P/NF	2, 4-DCP	100%	0.0362	–	60	–	[69]
Pd/Fe-NiO/NF	2, 4-D	100%	–	0.76 min⁻¹·g⁻¹	4.09	–	[54]
Pd-Co₃O₄/Ni foam electrode	2, 4-D	94.2%	–	–	12.1	–	[71]
TiN-Pd	2, 4-DCP	96.4%	0.0146	–	52	1116	[16]
Pd/Co-MNSs/Ni foam	CAP	~97%	0.11	–	–	–	[76]
C-Ag₃₂Pd₆₈	2, 4-DCP	100%	–	2.58 min⁻¹·g⁻¹	~32%	–	[24]
Pd₇Au₃ ANs	4-CP	98.35%	0.017	–	14%	–	[43]
Pd/amine	2, 4-DCP	89.3%	–	2.32 min⁻¹·g⁻¹	–	–	[80]
Pd/C-PEG25	2, 4-DCP	100%	0.004	2.13 min⁻¹·g⁻¹	11.7%	–	[81]
Pd Cube-S	2-CP	80%	0.00458	–	20.4%	4.32	[40]
N/G-430-Pd	2, 4-DCP	76.45%	–	0.28 min⁻¹·g⁻¹	＜28%	–	[34]
Pd/NCMK-3-200	2, 4-DCP	~80%	–	3.37 min⁻¹·g⁻¹	–	19.8	[3]
Pd NPs/NO-C	CAP	99%	0.1036	–	–	6.72	[82]
Pd/PANI-rGO/NF	DCF	99.3%	0.028	–	–	–	[83]
Pd/NiCo-MOF/Nickel foam	CAP	100%	0.07	–	11.82%	–	[53]
Pd/MXene@Ni-MOF/NF	2-CP	100%	0.065	–	–	–	[84]
Pd/NiCo-LDH/NF	2, 4-DCP	94.81%	0.0164	32.80 min⁻¹·g⁻¹	–	–	[41]
Pd/Ni₂P-Ni foam	4-CP	100%	–	–	22.62%	–	[48]
NiFeP-Ti₃C₂T_x	4-CP	100%	0.04	446.01 min⁻¹·g⁻¹	–	–	[45]
Pd/NiCo₂O₄/Ni-foam	2, 4-D	100%	–	–	5.2%	–	[85]
Pd@Co₃O_4-OV/NF	2, 4-DCP	95.4%	0.034	–	–	–	[86]
TiC-Pd/Ni foam	2, 4-DCBA	100%	0.039	–	–	–	[87]
Pd/TiC/Ti	2, 4-DCBA	78%	0.003	–	–	–	[29]
Pd/STO	2, 4-DCP	80%	–	6.38 min⁻¹·g⁻¹	33%	–	[88]
Pd-Mn/Ni foam	2, 4-DCP	100%	0.0357	9.58 min⁻¹·g⁻¹	29.11%	–	[89]
Pd/MnO₂/Ni foam	2, 4-DCBA	100%	0.049	2.83 min⁻¹·g⁻¹	–	–	[25]
Pd/MnO₂-Ni foam	2, 4-DCP	100%	–	8.29 min⁻¹·g⁻¹	23%	–	[15]
Pd-TiO₂	2, 4-DCP	80%	–	–	–	1.68	[32]
Pd-PCN	2, 4-DCP	87%	0.68	–	–	–	[1]
Pd/P-PCN	2, 4-DCP	82.5%	0.172	–	–	–	[62]
PdNi/NPCNs	4-CP	100%	0.023	–	25.8%	9	[2]
Pd-Ni/MWCNTs/GF	4-CP	100%	0.162	–	–	–	[90]
Cu@Pd/Ti electrode	atrazine	91.5%	0.0214	–	–	–	[91]
Pd-Cu@MXene/CC	DCF	93.3 ± 0.1%	0.0057	–	–	–	[92]
Pd_0.5Fe_0.5/graphene	CPs	–	–	–	–	–	[93]
Co-SG	2, 4-DCBA	91.1%	–	–	–	–	[94]
Ni-WC/NF	4-CP	100%	0.022	–	13.9%	–	[33]
CoPO/GC/NF	2, 4-D	84.0%	0.0087	–	–	–	[95]

表1

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图32

表2

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Catalysts for electrocatalytic dechlorination of chlorinated aromatic hydrocarbons: synthetic strategies, applications, and challenges

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