Efficient Solar-Driven Water Splitting Enabled by Perovskite Photovoltaics and a Halogen-Modulated Metal-Organic Framework Electrocatalyst

Xintong Li; Xin Wu; Bo Li; Shoufeng Zhang; Yizhe Liu; Zhen Li; Dong Zhang; Xue Wang; Qidi Sun; Danpeng Gao; Chunlei Zhang; Wei-Hsiang Huang; Chu-Chen Chueh; Chi-Liang Chen; Shangfeng Yang; Shuang Xiao; Zilong Wang; Zonglong Zhu

doi:10.1021/acsnano.3c05583

Efficient Solar-Driven Water Splitting Enabled by Perovskite Photovoltaics and a Halogen-Modulated Metal-Organic Framework Electrocatalyst

ACS Nano. 2023 Dec 12;17(23):23478-23487. doi: 10.1021/acsnano.3c05583. Epub 2023 Nov 27.

Authors

Xintong Li¹, Xin Wu¹, Bo Li¹, Shoufeng Zhang¹, Yizhe Liu¹, Zhen Li¹, Dong Zhang¹, Xue Wang^{2

3}, Qidi Sun¹, Danpeng Gao¹, Chunlei Zhang¹, Wei-Hsiang Huang^{4

5}, Chu-Chen Chueh⁶, Chi-Liang Chen⁵, Shangfeng Yang³, Shuang Xiao⁷, Zilong Wang⁸, Zonglong Zhu^{1

9}

Affiliations

¹ Department of Chemistry, City University of Hong Kong, Kowloon 999077, Hong Kong.
² Department of Materials Science and Engineering, City University of Hong Kong, Kowloon 999077, Hong Kong.
³ CAS Key Laboratory of Materials for Energy Conversion, Anhui Laboratory of Advanced Photon Science and Technology, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China.
⁴ Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology (NTUST), Taipei 10607, Taiwan.
⁵ National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan, ROC.
⁶ Department of Chemical Engineering, National Taiwan University, Taipei 10617, Taiwan.
⁷ Center for Advanced Material Diagnostic Technology and College of Engineering Physics, Shenzhen Technology University, Shenzhen 518118, P. R. China.
⁸ Siyuan Laboratory, Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University, Guangzhou, Guangdong 510632, P. R. China.
⁹ City University of Hong Kong Shenzhen Research Institute, Shenzhen, Guangdong 518057, China.

PMID: 38009599
DOI: 10.1021/acsnano.3c05583

Abstract

Solar-driven water splitting powered by photovoltaics enables efficient storage of solar energy in the form of hydrogen fuel. In this work, we demonstrate efficient solar-to-hydrogen conversion using perovskite (PVK) tandem photovoltaics and a halogen-modulated metal-organic framework (MOF) electrocatalyst. By substituting tetrafluoroterephthalate (TFBDC) for terephthalic (BDC) ligands in a nickel-based MOF, we achieve a 152 mV improvement in oxygen evolution reaction (OER) overpotential at 10 mA·cm². Through X-ray photoelectron spectroscopy (XPS), X-ray adsorption structure (XAS) analysis, theoretical simulation, and electrochemical results, we demonstrated that the introduction of fluorine atoms enhanced the intrinsic activity of Ni sites as well as the transfer property and accessibility of the MOF. Using this electrocatalyst in a bias-free photovoltaic electrochemical (PV-EC) system with a PVK/organic tandem solar cell, we achieve 6.75% solar-to-hydrogen efficiency (η_STH). We also paired the electrocatalyst with a PVK photovoltaic module to drive water splitting at 206.7 mA with η_STH of 10.17%.

Keywords: ligand engineering; metal−organic framework; oxygen evolution; solar-to-hydrogen efficiency; water splitting.