TY - JOUR
T1 - Structurally disordered CoSx–Co(OH)2 heterointerface for boosting alkaline hydrogen evolution reaction
AU - Dai, Yulong
AU - Tang, Qinshan
AU - Hu, Yuanxiao
AU - Guo, Xinkai
AU - Ma, Guoxin
AU - Jin, Rui
AU - Zhu, Xiaoyu
AU - Liu, Jia
AU - Xu, Li
AU - Li, Siwei
AU - Khalafallah, Diab
AU - Liu, Zhe
N1 - Publisher Copyright:
© 2026 Elsevier Inc.
PY - 2026/7
Y1 - 2026/7
N2 - The kinetics of the hydrogen evolution reaction (HER) process in alkaline media are inherently slower than in acidic media, resulting in a significant need for high-performance, durable, and cost-effective electrocatalysts. Structurally disordered heterostructure nanomaterials bring together the advantages of disordered and composite materials. Accordingly, this study demonstrates a structurally disordered cobalt sulfide/hydroxide (CoSx-Co(OH)2) heterostructure framework with an intimate interface between two distinct phases, establishing a highly active environment. The heterostructure catalyst is in situ coated on a three-dimensional (3D) microporous Cu foam (CF) skeleton using a one-step electrodeposition approach at a high cathodic current. The intimate, binder-free electrical connection between active components and highly conductive 3D Cu scaffold dramatically decreases interfacial resistance and promotes rapid electron penetration throughout the catalyst system. Consequently, the CoSx-Co(OH)2/CF catalyst acquires a current density of 10 mA cm−2 at an overpotential of 88 mV vs. RHE in a 1 M KOH, markedly surpassing Co(OH)2. Besides, it displays a favorable Tafel slope of 81.1 mV dec−1, low charge-transfer resistance, an enlarged electrochemically active surface area, and exceptional durability for 1000 cycles and 500 h of continuous operation. In addition to half-cell tests, a compact zero-gap alkaline electrolyzer, utilizing the CoSx-Co(OH)2/CF cathode and NiFe LDH anode, exhibits stable operation at 500 mA cm−2 at 60 °C for ⁓240 h, indicating the practical feasibility. Density functional theory (DFT) calculation results suggest that the heterointerface generates a robust built-in electric field, facilitating the electron transport from CoSx to Co(OH)2, downshifting the Co d-band center, and enhancing the Gibbs free energy of hydrogen adsorption (ΔGH*). The resultant “adsorb–dissociate–desorb” synergy, where water dissociation is promoted on Co(OH)2 and H* conversion is strengthened on CoSx, verifies the expedited kinetics of alkaline HER. Therefore, this synergistic integration offers a versatile platform for regulating active sites accessibility, combining high catalytic reactivity and exceptional durability throughout economical, non-precious metal schemes.
AB - The kinetics of the hydrogen evolution reaction (HER) process in alkaline media are inherently slower than in acidic media, resulting in a significant need for high-performance, durable, and cost-effective electrocatalysts. Structurally disordered heterostructure nanomaterials bring together the advantages of disordered and composite materials. Accordingly, this study demonstrates a structurally disordered cobalt sulfide/hydroxide (CoSx-Co(OH)2) heterostructure framework with an intimate interface between two distinct phases, establishing a highly active environment. The heterostructure catalyst is in situ coated on a three-dimensional (3D) microporous Cu foam (CF) skeleton using a one-step electrodeposition approach at a high cathodic current. The intimate, binder-free electrical connection between active components and highly conductive 3D Cu scaffold dramatically decreases interfacial resistance and promotes rapid electron penetration throughout the catalyst system. Consequently, the CoSx-Co(OH)2/CF catalyst acquires a current density of 10 mA cm−2 at an overpotential of 88 mV vs. RHE in a 1 M KOH, markedly surpassing Co(OH)2. Besides, it displays a favorable Tafel slope of 81.1 mV dec−1, low charge-transfer resistance, an enlarged electrochemically active surface area, and exceptional durability for 1000 cycles and 500 h of continuous operation. In addition to half-cell tests, a compact zero-gap alkaline electrolyzer, utilizing the CoSx-Co(OH)2/CF cathode and NiFe LDH anode, exhibits stable operation at 500 mA cm−2 at 60 °C for ⁓240 h, indicating the practical feasibility. Density functional theory (DFT) calculation results suggest that the heterointerface generates a robust built-in electric field, facilitating the electron transport from CoSx to Co(OH)2, downshifting the Co d-band center, and enhancing the Gibbs free energy of hydrogen adsorption (ΔGH*). The resultant “adsorb–dissociate–desorb” synergy, where water dissociation is promoted on Co(OH)2 and H* conversion is strengthened on CoSx, verifies the expedited kinetics of alkaline HER. Therefore, this synergistic integration offers a versatile platform for regulating active sites accessibility, combining high catalytic reactivity and exceptional durability throughout economical, non-precious metal schemes.
KW - CoS-Co(OH)
KW - Electrodeposition
KW - Heterointerface engineering
KW - Hydrogen evolution reaction
KW - Structurally disordered
KW - Zero-gap electrolyzer
UR - https://www.scopus.com/pages/publications/105030922941
U2 - 10.1016/j.jcis.2026.140148
DO - 10.1016/j.jcis.2026.140148
M3 - 文章
C2 - 41747581
AN - SCOPUS:105030922941
SN - 0021-9797
VL - 713
JO - Journal of Colloid and Interface Science
JF - Journal of Colloid and Interface Science
M1 - 140148
ER -