In-Situ-Grown Cu Dendrites Plasmonically Enhance Electrocatalytic Hydrogen Evolution on Facet-Engineered Cu2O,Advanced Materials

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In-Situ-Grown Cu Dendrites Plasmonically Enhance Electrocatalytic Hydrogen Evolution on Facet-Engineered Cu2O
Advanced Materials ( IF 27.4 ) Pub Date : 2023-09-04 , DOI: 10.1002/adma.202305742
Hao Zhang _{1,

2} , Jiefeng Diao ₃ , Yonghui Liu ₄ , Han Zhao ₅ , Bryan K Y Ng ₆ , Zhiyuan Ding ₇ , Zhenyu Guo ₈ , Huanxin Li ₉ , Jun Jia ₄ , Chang Yu ₁₀ , Fang Xie ₁ , Graeme Henkelman ₃ , Maria-Magdalena Titirici ₈ , John Robertson _{4,

9} , Peter Nellist ₇ , Chunying Duan ₁₁ , Yuzheng Guo ₄ , D Jason Riley ₁ , Jieshan Qiu ₁₀

Affiliation

Department of Materials and London Center for Nanotechnology, Imperial College London, London, SW7 2AZ, UK.
Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford, OX1 3TA, UK.
Department of Chemistry and the Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, TX, 78712, USA.
School of Electrical Engineering and Automation, Wuhan University, Wuhan, 430072, P. R. China.
Department of Chemistry, University of Zurich, Winterthurerstrasse 190, Zurich, CH-8057, Switzerland.
Wolfson Catalysis Centre, Department of Chemistry, University of Oxford, Oxford, OX1 3QR, UK.
Department of Materials, University of Oxford, Oxford, OX1 3PH, UK.
Department of Chemical Engineering, Imperial College London, London, SW7 2AZ, UK.
Department of Engineering, University of Cambridge, Cambridge, CB2 1PZ, UK.
State Key Lab of Fine Chemicals, School of Chemical Engineering, Liaoning Key Lab for Energy Materials and Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
School of Chemistry, Dalian University of Technology, Dalian, Liaoning, 116024, P. R. China.

Herein, facet-engineered Cu₂O nanostructures are synthesized by wet chemical methods for electrocatalytic HER, and it is found that the octahedral Cu₂O nanostructures with exposed crystal planes of (111) (O-Cu₂O) has the best hydrogen evolution performance. Operando Raman spectroscopy and ex-situ characterization techniques showed that Cu₂O is reduced during HER, in which Cu dendrites are grown on the surface of the Cu₂O nanostructures, resulting in the better HER performance of O-Cu₂O after HER (O-Cu₂O-A) compared with that of the as-prepared O-Cu₂O. Under illumination, the onset potential of O-Cu₂O-A is ca. 52 mV positive than that of O-Cu₂O, which is induced by the plasmon-activated electrochemical system consisting of Cu₂O and the in-situ generated Cu dendrites. Incident photon-to-current efficiency (IPCE) measurements and the simulated UV–Vis spectrum demonstrate the hot electron injection (HEI) from Cu dendrites to Cu₂O. Ab initio nonadiabatic molecular dynamics (NAMD) simulations revealed the transfer of photogenerated electrons (27 fs) from Cu dendrites to Cu₂O nanostructures is faster than electron relaxation (170 fs), enhancing its surface plasmons activity, and the HEI of Cu dendrites increases the charge density of Cu₂O. These make the energy level of the catalyst be closer to that of H⁺/H₂, evidenced by the plasmon-enhanced HER electrocatalytic activity.

中文翻译：

原位生长的铜枝晶等离子体增强小面工程 Cu2O 上的电催化析氢

本文通过湿化学方法合成了用于电催化HER的小面工程Cu ₂ O纳米结构，发现具有暴露的(111)(O-Cu ₂ O)晶面的八面体Cu 2 O纳米结构具有最佳的析氢性能_。表现。Operando拉曼光谱和异位表征技术表明，Cu ₂ O在HER过程中被还原，其中Cu枝晶在Cu ₂ O纳米结构的表面生长，导致O-Cu ₂ O在HER后具有更好的HER性能（ O-Cu ₂ O-A)与所制备的O-Cu _{2 O相比。在光照下，O-Cu}₂ O-A的起始电位约为。_{比O-Cu 2} O正52 mV ，这是由Cu ₂ O和原位生成的Cu枝晶组成的等离激元激活电化学系统引起的。入射光子电流效率 (IPCE) 测量和模拟的紫外-可见光谱证明了从 Cu 枝晶到 Cu 2 O 的热电子注入 (HEI)。从头算非绝热分子动力学 (NAMD) 模拟揭示了光生电子的_转移（从Cu枝晶到Cu _{2 O纳米结构的电子弛豫(170 fs)速度比电子弛豫(170 fs)更快，增强了其表面等离子体活性，并且Cu枝晶的HEI增加了Cu}₂ O的电荷密度。这些使得催化剂的能级更接近H ⁺ /H ₂，由等离子体增强的HER电催化活性证明。

更新日期：2023-09-04

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