Cooperative alkaline hydrogen evolution via inducing local electric field and electron localization

doi:10.1016/S1872-2067(23)64532-2

Chinese Journal of Catalysis ›› 2023, Vol. 54: 229-237.DOI: 10.1016/S1872-2067(23)64532-2

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Cooperative alkaline hydrogen evolution via inducing local electric field and electron localization

Qiyou Wang^a^,^b^,¹, Yujie Gong^a^,¹, Yao Tan^b, Xin Zi^b, Reza Abazari^c, Hongmei Li^b, Chao Cai^b, Kang Liu^b, Junwei Fu^b, Shanyong Chen^d, Tao Luo^b, Shiguo Zhang^e, Wenzhang Li^d, Yifa Sheng^a, Jun Liu^a^,^*(), Min Liu^b^,^*()

^aSchool of Electrical Engineering, University of South China, Hengyang 421001, Hunan, China
^bHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha 410083, Hunan, China
^cDepartment of Chemistry, University of Maragheh, P.O. Box 55181-83111, Maragheh, Iran
^dCollege of Chemistry and Chemical Engineering, Central South University, Changsha 410083, Hunan, China
^eCollege of Materials Science and Engineering, Hunan University, Changsha 410082, Hunan, China

Received:2023-08-17 Accepted:2023-10-10 Online:2023-11-18 Published:2023-11-15
Contact: *E-mail: 2021000103@usc.edu.cn (J. Liu), minliu@csu.edu.cn (M. Liu).
About author:¹Contributed equally to this work.
Supported by:
Hunan Provincial Natural Science Foundation of China(2023JJ30499);Guangdong Provincial Natural Science Foundation of China(2022A1515010198);Natural Science Foundation of China(22002189);Natural Science Foundation of China(52202125);Natural Science Foundation of China(22376222);Central South University Research Programme of Advanced Interdisciplinary Studies(2023QYJC012);Central South University Innovation-Driven Re-search Programme(2023CXQD042)

Abstract

Abstract:

Alkaline hydrogen evolution reaction (HER) represents a promising means to store intermittent renewable energy into clean energy. Unfortunately, the sluggish H₂O dissociation and difficult *H adsorption-desorption are prominent obstacles to the development of alkaline HER. Herein, we developed a cooperative strategy via nanoneedle inducing local electric field and atomic doping causing electron localization for alkaline HER based on the preparation of Cu doped CoS₂ nanoneedles (Cu-CoS₂ NNs). Finite element method simulations and density functional theorycalculations demonstrate the local electric field accelerates H₂O dissociation and electron localization facilitates *H adsorption, respectively. In situ attenuated total reflection infrared spectroscopy and electro-response measurement experimentally reveal the superior ability to H₂O dissociation and *H adsorption for Cu-CoS₂ NNs. As a result, the Cu-CoS₂ NNs exhibit an ultralow overpotential of 64 mV at -10 mA cm^-2 and long-term stability over 100 h at -100 mA cm^-2 during alkaline HER, which outperforms most electrocatalysts in recently published works.

Key words: Alkaline hydrogen evolution, Local electric field, Electron localization, Cu doping, CoS₂ nanoneedles

Qiyou Wang, Yujie Gong, Yao Tan, Xin Zi, Reza Abazari, Hongmei Li, Chao Cai, Kang Liu, Junwei Fu, Shanyong Chen, Tao Luo, Shiguo Zhang, Wenzhang Li, Yifa Sheng, Jun Liu, Min Liu. Cooperative alkaline hydrogen evolution via inducing local electric field and electron localization[J]. Chinese Journal of Catalysis, 2023, 54: 229-237.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64532-2

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Figures/Tables 6

Fig. 1. Electric field distribution around the surface of HC-CoS2 (a) and LC-CoS2 (c). OH- concentration distributions around the surface of HC-CoS2 (b) and LC-CoS2 (d).

Fig. 2. Comparison of schematic diagram of electron localization for bare CoS2 (a) and Cu-CoS2 (b). Blue, cobalt; brown, copper; yellow, sulfur; white, hydrogen. (c) The charge density differences analysis. Green, depletion; red, accumulation. (d) PDOS and d-band center for Co. (e) Free energy diagram.

Fig. 3. (a) Schematic illustration of the preparation for catalysts. SEM images of Cu-CoS2 NNs (b) and Cu-CoS2 NWs (c). (d) HRTEM image of Cu-CoS2 NNs. TEM image of Cu-CoS2 NNs (e) and Cu-CoS2 NWs (f). (g) EDS mapping images of Cu-CoS2 NNs.

Fig. 4. High-resolution XPS of S 2p (a), Co 2p (b), and Cu 2p (c). (d) Cu LMM auger spectra.

Fig. 5. (a) OH- concentration on the surface of the catalysts at -0.07 V vs. RHE. In situ ATR-IR spectra of Cu-CoS2 NNs (b) and Cu-CoS2 NWs (c). (d) Current densities of Cu-CoS2 NNs (b) and Cu-CoS2 NWs electrodes in the electro-response measurements under Ar and H2.

Fig. 6. (a) HER polarization curves with a scan rate of 5 mV s-1 in 1.0 mol L-1 KOH solution. (b) Tafel plots originated from the corresponding polarization curves. (c) Overpotentials at a current density of -10 mA cm-2 and -100 mA cm-2. (d) Stability test at -0.18 V vs. RHE in 1.0 mol L-1 KOH solution. (e) Comparison of performance for different catalysts at a current density of -10 mA cm-2.

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Cooperative alkaline hydrogen evolution via inducing local electric field and electron localization

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