首页> 外文期刊>ACS catalysis >Unveiling the Bifunctional Photo/Electrocatalytic Activity of In Situ Grown CdSe QDs on g-C3N4 Nanosheet Z-Scheme Heterostructures for Efcient Hydrogen Generation
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Unveiling the Bifunctional Photo/Electrocatalytic Activity of In Situ Grown CdSe QDs on g-C3N4 Nanosheet Z-Scheme Heterostructures for Efcient Hydrogen Generation

机译:揭示原位生长的 CdSe 量子点在 g-C3N4 纳米片 Z 型异质结构上高效制氢的双功能光/电催化活性

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The successive ionic layer adsorption and reaction(SILAR)method was used to deposit several CdSe quantum dots(QDs)on the surface of g-C3N4 nanosheets.In comparison to the single moiety of g-C3N4,as-prepared heterostructures displayed an improved bifunctional photo-and electrocatalytic activity for oxygen(OER)and hydrogen evolution reactions(HER).Signifcantly,the 30 SILAR cycles optimized CdSe QDs/g-C3N4 heterostructure exhibited high performances and stabilities for the OER and HER reaction in alkaline conditions.The as-prepared heterostructure catalyst also exhibited an efcient photocatalytic activity toward the H2 evolution reaction and produced 4306 μmol of H2 gas with 23.8 of apparent quantum yield in the presence of triethanolamine as a sacrifcial agent.Photoluminescence spectros-copy,electron paramagnetic resonance,and impedance spectrosco-py suggest that the synergy between g-C3N4 nanosheets and CdSe QDs leads to higher catalytic activities,as indicated by the low overpotentials of 147 and 218 mV to obtain a 10 mA cm~(-2)current density for the HER and OER reactions,respectively.Furthermore,in situ Fourier transform infrared spectroscopy,liquid chromatography-mass spectroscopy,and high-performance liquid chromatography were conducted to determine the photochemical intermediate products to confrm the successful oxidation of TEOA by capturing holes.The outcome is in accordance with the fact that the photogenerated electrons are transferred from the conduction band(CB)of g-C3N4 nanosheets to the valence band(VB)of CdSe QDs in a Z-scheme manner.
机译:采用连续离子层吸附反应(SILAR)法在g-C3N4纳米片表面沉积了多个CdSe量子点(QDs)。与g-C3N4的单部分相比,异质结构对氧(OER)和析氢反应(HER)表现出更好的双功能光催化和电催化活性。值得注意的是,30个SILAR循环优化的CdSe QDs/g-C3N4异质结构在碱性条件下对OER和HER反应表现出较高的性能和稳定性。制备的异质结构催化剂对H2析出反应也表现出有效的光催化活性,在三乙醇胺作为牺牲剂存在下,产生了4306 μmol的H2气体,表观量子产率为23.8%。光致发光光谱复制、电子顺磁共振和阻抗光谱-py表明,g-C3N4纳米片和CdSe量子点之间的协同作用导致了更高的催化活性,147和218 mV的低过电位表明,HER和OER反应的电流密度分别为10 mA cm~(-2)。此外,还采用原位傅里叶变换红外光谱、液相色谱-质谱和高效液相色谱法测定光化学中间产物,以通过捕获孔洞成功氧化TEOA。结果符合光生电子以Z方案方式从g-C3N4纳米片的导带(CB)转移到CdSe量子点的价带(VB)的事实。

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