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Defects-engineered tailoring of tri-doped interlinked metal-free bifunctional catalyst with lower gibbs free energy of OER/HER intermediates for overall water splitting
Authors:G. Yasin  S. Ibraheem  S. Ali  M. Arif  S. Ibrahim  R. Iqbal  A. Kumar  M. Tabish  M.A. Mushtaq  A. Saad  H. Xu  W. Zhao
Affiliation:1. Institute for Advanced Study, Shenzhen University, Shenzhen 518060, Guangdong, China;2. College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, Guangdong, China;3. Department of Physics, Southern University of Science and Technology, Shenzhen 518055, China;4. Institute of Advanced Synthesis, Northwestern Polytechnical University, Xi''an 710072, China;5. College of Life Science and Technology, Beijing University of Chemical Technology, Beijing 100029, China;6. Nano-Technology Research Laboratory, Department of Chemistry, GLA University, Mathura, Uttar Pradesh 281406, India;7. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Abstract:Controllable tailoring of metal-free/carbon-based nanostructures tends an encouraging way to enhance the bifunctional activity of electrodes, but a great challenge owing to the sluggish kinetics of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). Herein, a facile tempted-defects assisted fractionation strategy is presented to synthesize N, S, and O tri-doped metal-free catalyst (DE-TDAP). Due to this effective tempted-defects and heteroatoms interlinking in DE-TDAP, it delivers the lowest overpotential toward both the OER (346 mV) and HER (154 mV) at 10 mA cm?2. Remarkably, the DE-TDAP-electrode carries only a cell voltage of 1.81 V at 10 mA cm?2 for overall water splitting and long-term stability. Considerably, the density functional theory (DFT) calculation exposes that the tailored-defects in tri-doped interlinking could enhance bifunctional catalytic performance devising from lower Gibbs free energy of OER/HER intermediates on active sites. This struggle henceforth provides a perceptive understanding of the synergetic principles of heteroatom-interlinking-tailoring nanostructures in water splitting.
Keywords:Metal-free catalyst  Heteroatom-interlinking-tailoring  Defect-engineering  Overall water splitting  DFT
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