电催化尿素氧化(UOR)替代动力学缓慢的析氧反应(OER)为高效制氢提供了新的思路。本研究通过简单的二次水热法制备了三维Ni_(3)S_(2)/NF微球催化剂(3D-Ni_(3)S_(2)/NF),由于独特的3D结构为UOR提供了高度开放的活性区域,并加快了电荷转移...电催化尿素氧化(UOR)替代动力学缓慢的析氧反应(OER)为高效制氢提供了新的思路。本研究通过简单的二次水热法制备了三维Ni_(3)S_(2)/NF微球催化剂(3D-Ni_(3)S_(2)/NF),由于独特的3D结构为UOR提供了高度开放的活性区域,并加快了电荷转移速率,3D-Ni_(3)S_(2)/NF表现出明显优于1D,2D-Ni_(3)S_(2)/NF电催化氧化尿素的活性。在1 mol L^(-1)KOH+0.33 mol L^(-1)尿素电解质溶液,3D-Ni_(3)S_(2)/NF电催化尿素氧化达到100 mA cm^(-2)的电流密度的电位仅需1.38 V vs.RHE,比OER电位减少了250 mV,同时在24 h稳定性测试中表现出良好的耐久性。此外,全尿素辅助制氢只需1.66 V即可达到50 mA cm^(-2),表现出比传统电解水(1.86 V)更低的电位。展开更多
A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of c...A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn–Ca–Al catalysts, according to the time dependences of reaction intermediates and products.展开更多
文摘电催化尿素氧化(UOR)替代动力学缓慢的析氧反应(OER)为高效制氢提供了新的思路。本研究通过简单的二次水热法制备了三维Ni_(3)S_(2)/NF微球催化剂(3D-Ni_(3)S_(2)/NF),由于独特的3D结构为UOR提供了高度开放的活性区域,并加快了电荷转移速率,3D-Ni_(3)S_(2)/NF表现出明显优于1D,2D-Ni_(3)S_(2)/NF电催化氧化尿素的活性。在1 mol L^(-1)KOH+0.33 mol L^(-1)尿素电解质溶液,3D-Ni_(3)S_(2)/NF电催化尿素氧化达到100 mA cm^(-2)的电流密度的电位仅需1.38 V vs.RHE,比OER电位减少了250 mV,同时在24 h稳定性测试中表现出良好的耐久性。此外,全尿素辅助制氢只需1.66 V即可达到50 mA cm^(-2),表现出比传统电解水(1.86 V)更低的电位。
基金Supported by the Changcheng Scholars Program of Beijing(CIT&TCD 20150316)
文摘A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn–Ca–Al catalysts, according to the time dependences of reaction intermediates and products.
