Dual Active Center-Assembled Cu31S16–Co9-xNixS8 Heterodimers: Coherent Interface Engineering Induces Multihole Accumulation for Light-Enhanced Electrocatalytic Oxygen Evolution
| Autor: | Gaofei Hu, Leyu Wang, Renjie Wu, Yueguang Chen, Jiabin Cui, Xintian Liu |
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| Rok vydání: | 2021 |
| Předmět: |
Materials science
Oxygen evolution 02 engineering and technology Overpotential 010402 general chemistry 021001 nanoscience & nanotechnology Electrochemistry Electrocatalyst 01 natural sciences Nanomaterial-based catalyst 0104 chemical sciences Chemical physics Hydrogen fuel Water splitting General Materials Science Charge carrier 0210 nano-technology |
| Zdroj: | ACS Applied Materials & Interfaces. 13:20094-20104 |
| ISSN: | 1944-8252 1944-8244 |
| DOI: | 10.1021/acsami.1c02353 |
| Popis: | The design of low-cost yet highly efficient electrocatalysts plays a critical role in energy storage and conversion reactions. The oxygen evolution reaction (OER) is considered a bottleneck of electrochemical water splitting for hydrogen fuel generation. It is still challenging to extract a high density of charge carriers in noble-metal-free alternative catalysts to facilitate sluggish kinetics. Herein, we report the rational design and coherent interface engineering for combining light-harvesting Cu31S16 with electroactive Co9-xNixS8 (x = 0-9) to form novel Cu31S16-Co9-xNixS8 heterodimers. By delicately controlling the kinetic growth in a seed-mediated growth method, the bifunctional centers, even with two distinct crystal phases, were integrated into a synergistic architecture, which achieved full-spectrum solar energy capture and light conversion to drive and activate the electrochemical reaction. Benefiting from the well-defined structure, high-quality interface, oriented attachment, and optimal Co/Ni bimetal ratio, Cu31S16-Co7.2Ni1.8S8 produces a dramatically reduced overpotential (242 mV at 10 mA cm-2) with a shift of 83 mV under visible-light excitation, achieving a 4.5-fold higher turnover frequency than that of its unirradiated Co7.2Ni1.8S8 counterpart. This enhanced performance also far exceeds commercial RuO2 (358 mV at 10 mA cm-2) and most nonprecious-metal nanocatalysts. Further mechanistic studies reveal that coherent interface engineering leads to a strong photo/electricity coupling effect and efficient spatial charge separation, which induces sufficient hot holes that eventually accumulate at the electroactive sites to accelerate the multihole-involved OER. This work would open up new opportunities for the fabrication of non-noble metal electrocatalysts and management of charge carriers. |
| Databáze: | OpenAIRE |
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