Electrocatalytic Coenhancement of Bimetallic Polyphthalocyanine-Anchored Ru Nanoclusters Enabling Efficient Overall Water Splitting at Ampere-Level Current Densities

被引:15
作者
Chen, Hao [1 ]
Ding, Rong [1 ]
Liu, Bo-Wen [1 ]
Zeng, Fu-Rong [1 ]
Zhao, Hai-Bo [1 ]
机构
[1] Sichuan Univ, Coll Chem, Collaborat Innovat Ctr Ecofriendly & Fire Safety P, Natl Engn Lab Ecofriendly Polymer Mat Sichuan, 24 South Sect 1,Yihuan Rd, Chengdu 610064, Sichuan, Peoples R China
基金
中国国家自然科学基金;
关键词
electrocatalytic coenhancement; industrial conditions; metal polyphthalocyanine; overall water splitting; ultrafine clusters; HYDROGEN EVOLUTION;
D O I
10.1002/smll.202306274
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Efficient electrocatalysts capable of operating continuously at industrial ampere-level current densities are crucial for large-scale applications of electrocatalytic water decomposition for hydrogen production. However, long-term industrial overall water splitting using a single electrocatalyst remains a major challenge. Here, bimetallic polyphthalocyanine (FeCoPPc)-anchored Ru nanoclusters, an innovative electrocatalyst comprising the hydrogen evolution reaction (HER) active Ru and the oxygen evolution reaction (OER) active FeCoPPc, engineered for efficient overall water splitting are demonstrated. By density functional theory calculations and systematic experiments, the electrocatalytic coenhancement effect resulting from unique charge redistribution, which synergistically boosts the HER activity of Ru and the OER activity of FeCoPPc by optimizing the adsorption energy of intermediates, is unveiled. As a result, even at a large current density of 2.0 A cm-2, the catalyst exhibits low overpotentials of 220 and 308 mV, respectively, for HER and OER. It exhibits excellent stability, requiring only 1.88 V of cell voltage to achieve a current density of 2.0 A cm-2 in a 6.0 m KOH electrolyte at 70 & DEG;C, with a remarkable operational stability of over 100 h. This work provides a new electrocatalytic coenhancement strategy for the design and synthesis of electrocatalyst, paving the way for industrial-scale overall water splitting applications. Here, an innovative electrocatalyst, bimetallic polyphthalocyanine (FeCoPPc)-anchored Ru nanoclusters, designed for efficient overall water splitting under industrial conditions is demonstrated. This electrocatalyst uses the unique electrocatalytic coenhancement effect, resulting from unique charge redistribution, optimizes the desorption of hydrogen by Ru in hydrogen evolution reaction process and reduces the energy barrier of OOH* formation, achieving outstanding industrial overall water splitting performance.image
引用
收藏
页数:10
相关论文
共 46 条
[1]   Efficacious Electrochemical Oxygen Evolution from a Novel Co(II) Porphyrin/Pyrene-Based Conjugated Microporous Polymer [J].
Bhunia, Subhajit ;
Bhunia, Kousik ;
Patra, Bidhan Chandra ;
Das, Sabuj Kanti ;
Pradhan, Debabrata ;
Bhaumik, Asim ;
Pradhan, Anirban ;
Bhattacharya, Santanu .
ACS APPLIED MATERIALS & INTERFACES, 2019, 11 (01) :1520-1528
[2]   Optimizing Hydrogen Binding on Ru Sites with RuCo Alloy Nanosheets for Efficient Alkaline Hydrogen Evolution [J].
Cai, Chao ;
Liu, Kang ;
Zhu, Yuanmin ;
Li, Pengcheng ;
Wang, Qiyou ;
Liu, Bao ;
Chen, Shanyong ;
Li, Huangjingwei ;
Zhu, Li ;
Li, Hongmei ;
Fu, Junwei ;
Chen, Yu ;
Pensa, Evangelina ;
Hu, Junhua ;
Lu, Ying-Rui ;
Chan, Ting-Shan ;
Cortes, Emiliano ;
Liu, Min .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (04)
[3]   Amorphous FeOOH Oxygen Evolution Reaction Catalyst for Photoelectrochemical Water Splitting [J].
Chemelewski, William D. ;
Lee, Heung-Chan ;
Lin, Jung-Fu ;
Bard, Allen J. ;
Mullins, C. Buddie .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (07) :2843-2850
[4]   Structural Transformation of Heterogeneous Materials for Electrocatalytic Oxygen Evolution Reaction [J].
Ding, Hui ;
Liu, Hongfei ;
Chu, Wangsheng ;
Wu, Changzheng ;
Xie, Yi .
CHEMICAL REVIEWS, 2021, 121 (21) :13174-13212
[5]   A One-Step Self-Flowering Method toward Programmable Ultrathin Porous Carbon-Based Materials for Microwave Absorption and Hydrogen Evolution [J].
Ding, Rong ;
Wang, Yan-Qin ;
Zeng, Fu-Rong ;
Liu, Bo-Wen ;
Wang, Yu-Zhong ;
Zhao, Hai-Bo .
SMALL, 2023, 19 (36)
[6]   Ultra-Small Face-Centered-Cubic Ru Nanoparticles Confined within a Porous Coordination Cage for Dehydrogenation [J].
Fang, Yu ;
Li, JiaLuo ;
Togo, Tatsuo ;
Jin, FangYing ;
Xiao, ZhiFeng ;
Liu, Lujia ;
Drake, Hannah ;
Lian, XiZhen ;
Zhou, Hong-Cai .
CHEM, 2018, 4 (03) :555-563
[7]   Understanding the Atomic and Defective Interface Effect on Ruthenium Clusters for the Hydrogen Evolution Reaction [J].
Gao, Taotao ;
Tang, Xiangmin ;
Li, Xiaoqin ;
Wu, Shuaiwei ;
Yu, Shumin ;
Li, Panpan ;
Xiao, Dan ;
Jin, Zhaoyu .
ACS CATALYSIS, 2023, 13 (01) :49-59
[8]   Supported Cobalt Polyphthalocyanine for High-Performance Electrocatalytic CO2 Reduction [J].
Han, Na ;
Wang, Yu ;
Ma, Lu ;
Wen, Jianguo ;
Li, Jing ;
Zheng, Hechuang ;
Nie, Kaiqi ;
Wang, Xinxia ;
Zhao, Feipeng ;
Li, Yafei ;
Fan, Jian ;
Zhong, Jun ;
Wu, Tianpin ;
Miller, Dean J. ;
Lu, Jun ;
Lee, Shuit-Tong ;
Li, Yanguang .
CHEM, 2017, 3 (04) :652-664
[9]   Recent progress made in the mechanism comprehension and design of electrocatalysts for alkaline water splitting [J].
Hu, Congling ;
Zhang, Lei ;
Gong, Jinlong .
ENERGY & ENVIRONMENTAL SCIENCE, 2019, 12 (09) :2620-2645
[10]   Regulating the Active Sites of Metal-Phthalocyanine at the Molecular Level for Efficient Water Electrolysis: Double Deciphering of Electron-Withdrawing Groups and Bimetallic [J].
Jiang, Ling ;
Gu, Mingzheng ;
Zhao, Shengrong ;
Wang, Hao ;
Huang, Xiaomin ;
Gao, An ;
Zhu, Huiling ;
Sun, Ping ;
Liu, Xudong ;
Lin, Haili ;
Zhang, Xiaojun .
SMALL, 2023, 19 (11)