The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu...The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.展开更多
在异丙醇水溶液中以钛酸丁酯为钛源,MoS2为敏化剂,硅藻土为负载剂,通过溶胶-凝胶法和水热法制备TiO2/MoS2@硅藻土的复合光催化剂。通过傅里叶红外光谱(FT-IR)、X射线衍射(XRD)、漫反射光谱(DRS)、扫描电镜(SEM)和N2吸附-脱附对催化剂组...在异丙醇水溶液中以钛酸丁酯为钛源,MoS2为敏化剂,硅藻土为负载剂,通过溶胶-凝胶法和水热法制备TiO2/MoS2@硅藻土的复合光催化剂。通过傅里叶红外光谱(FT-IR)、X射线衍射(XRD)、漫反射光谱(DRS)、扫描电镜(SEM)和N2吸附-脱附对催化剂组成、形貌及结构进行分析,以亚甲基蓝(MB)为降解有机污染物目标,降解MB溶液前后的浓度比值(ct/c0)为评价指标,对催化剂种类及催化剂的用量进行了优化研究。结果表明,TiO2/MoS2@硅藻土复合催化剂稳定性高,催化活性强,1 mg/mL该复合催化剂降解50 mL 3~10 mg/L的MB溶液,ct/c0值范围为0.015~0.048。降解过程符合一级反应动力学Langmuir-Hinshelwood方程。展开更多
基金supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972)China Postdoctoral Science Foundation(2022M722867)Key Research Project of Higher Education Institutions in Henan Province(23A530001)。
文摘The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.
基金Project(2021YFA1401300)supported by the National Key Research and Development Program of ChinaProject(2021RC3021)supported by the Science and Technology Innovation Program of Hunan Province,ChinaProject(2021JJ40780)supported by the Natural Science Foundation of Hunan Province,China。
文摘在异丙醇水溶液中以钛酸丁酯为钛源,MoS2为敏化剂,硅藻土为负载剂,通过溶胶-凝胶法和水热法制备TiO2/MoS2@硅藻土的复合光催化剂。通过傅里叶红外光谱(FT-IR)、X射线衍射(XRD)、漫反射光谱(DRS)、扫描电镜(SEM)和N2吸附-脱附对催化剂组成、形貌及结构进行分析,以亚甲基蓝(MB)为降解有机污染物目标,降解MB溶液前后的浓度比值(ct/c0)为评价指标,对催化剂种类及催化剂的用量进行了优化研究。结果表明,TiO2/MoS2@硅藻土复合催化剂稳定性高,催化活性强,1 mg/mL该复合催化剂降解50 mL 3~10 mg/L的MB溶液,ct/c0值范围为0.015~0.048。降解过程符合一级反应动力学Langmuir-Hinshelwood方程。
基金Supported by National Natural Science Foundation of China (50741003)Key Project of Science and Technology of Ministry of Education of China (107066)Anhui Provincial Natural Science Foundation (070414181)
