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Browsing by Author "Huang, Haoliang"

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  • Gold Single Atom Doped Defective Nanoporous Copper Octahedrons for Electrocatalytic Reduction of Carbon Dioxide to Ethylene
    Publication . Zhao, Yang; Wang, Yanan; Yu, Zhipeng; Song, Chao; Wang, Jingwei; Huang, Haoliang; Meng, Lijian; Liu, Miao; Liu, Lifeng
    Electrocatalytic CO2 reduction into high-value multicarbon products offers a sustainable approach to closing the anthropogenic carbon cycle and contributing to carbon neutrality, particularly when renewable electricity is used to power the reaction. However, the lack of efficient and durable electrocatalysts with high selectivity for multicarbons severely hinders the practical application of this promising technology. Herein, a nanoporous defective Au1Cu single-atom alloy (DeAu1Cu SAA) catalyst is developed through facile low-temperature thermal reduction in hydrogen and a subsequent dealloying process, which shows high selectivity toward ethylene (C2H4), with a Faradaic efficiency of 52% at the current density of 252 mA cm−2 under a potential of −1.1 V versus reversible hydrogen electrode (RHE). In situ spectroscopy measurements and density functional theory (DFT) calculations reveal that the high C2H4 product selectivity results from the synergistic effect between Au single atoms and defective Cu sites on the surface of catalysts, where Au single atoms promote *CO generation and Cu defects stabilize the key intermediate *OCCO, which altogether enhances C−C coupling kinetics. This work provides important insights into the catalyst design for electrochemical CO2 reduction to multicarbon products.
    2025Journal article Open access Show more
  • Sulfur and phosphorus co-doped FeCoNiCrMn high-entropy alloys as efficient sulfion oxidation reaction catalysts enabling self-powered asymmetric seawater electrolysis
    Publication . Yu, Zhipeng; Boukhvalov, Danil W.; Tan, Hao; Xiong, Dehua; Feng, Chuangshi; Wang, Jingwei; Wang, Wei; Zhao, Yang; Xu, Kaiyang; Su, Weifeng; Xiang, Xinyi; Lin, Fei; Huang, Haoliang; Zhang, Fuxiang; Zhang, Lei; Meng, Lijian; Liu, Lifeng
    Seawater electrolysis (SWE) represents a promising approach to green hydrogen (H2) production but currently faces substantial challenges such as the interference of chlorine chemistry and high energy consumption. In this work, we demonstrate that by replacing the energy-demanding oxygen evolution reaction (OER) with the sulfion oxidation reaction (SOR) and by implementing the concept of bipolar membrane (BPM) electrolysis in an acid-base dual electrolyte system, not only can the notorious chlorine evolution reaction (CER) be completely circumvented, but the energy consumption of SWE be significantly reduced. To do so, we develop a sulfur and phosphorus co-doped FeCoNiCrMn high entropy alloy (HEA-SP) catalyst, which shows good electrocatalytic performance for the SOR in alkaline-saline water. This can be attributed to the abundant lattice defects and strains in HEA-SP, leading to a high density of active sites and an optimized electronic structure favorable for the SOR. Moreover, density functional theory calculations and in situ Raman spectroscopy characterization reveal the crucial role of imperfect sulfur coverage on the HEA in facilitating the formation of Sx clusters during the SOR. Using the HEA-SP as anode catalysts, the SOR-assisted SWE only needs electrical energy of 0.253 kWh to produce one cubic meter of H2 at 100 mA cm−2, in the presence of a BPM. Impressively, chlorine-free H2 production from seawater and upgrading of sulfions to valuable sulfur can occur simultaneously and spontaneously at 10 mA cm−2, highlighting the great potential of the HEA-SP catalysts and the asymmetric cell design to enable energy- and cost-effective seawater electrolysis.
    2024Journal article Restricted access Show more