Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the develop...Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability.展开更多
锌配合物的绿色合成与表征是结合配合物基础知识和当前科学研究热点设计改进的一个综合性实验。本文以水为溶剂,以对氨基苯磺酸(4-ABS)和ZnO为主要原料,直接法制备得到一种三维网状配合物。对该配合物进行单晶X射线衍射、红外光谱、热...锌配合物的绿色合成与表征是结合配合物基础知识和当前科学研究热点设计改进的一个综合性实验。本文以水为溶剂,以对氨基苯磺酸(4-ABS)和ZnO为主要原料,直接法制备得到一种三维网状配合物。对该配合物进行单晶X射线衍射、红外光谱、热重分析、紫外以及荧光光谱等结构表征,并采用Materials Studio (MS)软件的CASTEP模块,对配合物的几何构型进行优化,从原子水平上进一步佐证配合物的最优结构及稳定化能。该实验过程包含配合物制备、蒸发浓缩、减压过滤、单晶培养、紫外及荧光光谱测试、热重分析、理论计算等,整个教学过程综合性及可操作性较强。同时,该实验把绿色合成融入到实验方案设计和实施的全过程,使学生树立节能环保的理念,激发学生探究真知的兴趣和热情,使其在加深理解配位化学基础知识的同时,获得了相关前沿热点知识,对培养学生创新思维、科学研究能力和综合素质具有十分重要的意义。展开更多
基金the financial support of Guangdong Basic and Applied Basic Research Foundation (No. 2023A1515010940)Shenzhen Natural Science Fund (the Stable Support Plan Program No. 20220809160022001)the Shenzhen Science and Technology Programs (No. ZDSYS20220527171401003, KQTD20190929173914967)。
文摘Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability.
文摘锌配合物的绿色合成与表征是结合配合物基础知识和当前科学研究热点设计改进的一个综合性实验。本文以水为溶剂,以对氨基苯磺酸(4-ABS)和ZnO为主要原料,直接法制备得到一种三维网状配合物。对该配合物进行单晶X射线衍射、红外光谱、热重分析、紫外以及荧光光谱等结构表征,并采用Materials Studio (MS)软件的CASTEP模块,对配合物的几何构型进行优化,从原子水平上进一步佐证配合物的最优结构及稳定化能。该实验过程包含配合物制备、蒸发浓缩、减压过滤、单晶培养、紫外及荧光光谱测试、热重分析、理论计算等,整个教学过程综合性及可操作性较强。同时,该实验把绿色合成融入到实验方案设计和实施的全过程,使学生树立节能环保的理念,激发学生探究真知的兴趣和热情,使其在加深理解配位化学基础知识的同时,获得了相关前沿热点知识,对培养学生创新思维、科学研究能力和综合素质具有十分重要的意义。
