摘要
Co(NO_(3))_(2)·6H_(2)O与钛酸四丁酯通过混合焙烧法得到了产物Co-TiO_(2),然后其与NaH_(2)PO_(2)按不同质量比混合研磨焙烧,制备了一系列过渡金属磷化物催化剂(CoP-TiO_(2))。采用SEM、TEM、XRD、XPS和UV-Vis DRS对催化剂的微观形貌和结构组成进行了表征。将CoP-TiO_(2)用于催化氨硼烷(AB)水解制氢,通过控制变量法,考察了m(NaH_(2)PO_(2))∶m(Co-TiO_(2))、有无可见光照、反应温度、AB浓度对CoP-TiO_(2)催化AB水解制氢性能的影响,并测试了催化剂在最佳反应条件下的循环稳定性。结果表明,由m(NaH_(2)PO_(2))∶m(Co-TiO_(2))=2∶1制备的催化剂2CoP-TiO_(2)表现出最佳的催化性能,在可见光照射、反应温度为298 K的条件下,20 mg 2CoP-TiO_(2)催化60 mL浓度为0.5 mol/L AB水溶液水解制氢,转化频率最高,为38.7 min^(-1),反应的活化能为46.4 kJ/mol。2CoP-TiO_(2)具有良好的循环稳定性,经过5次循环测试后,其催化AB水解制氢的反应时间没有明显增加。磷的引入降低了带隙能量,从Co-TiO_(2)的2.70 eV降至2CoP-TiO_(2)的2.46 eV,提高了电子迁移速率,从而促进了光催化反应的进行。
Co(NO_(3))_(2)·6H_(2)O was calcinated with tetrabutyl titanate to obtain product Co-TiO_(2),which was then mixed with NaH_(2)PO_(2)in different mass ratio to prepare a series of transition metal phosphide catalysts(CoP-TiO_(2))by grinding and calcination.The catalysts obtained were characterized by SEM,TEM,XRD,XPS and UV-Vis DRS for analysis on microstructure and composition,and used to catalyze the hydrolysis of ammonia borane(AB)for hydrogen production.The effects of m(NaH_(2)PO_(2))∶m(Co-TiO_(2)),visible light irradiation,reaction temperature and AB concentration on the catalytic performance of CoP-TiO_(2)for AB hydrolysis were investigated by control variable method,and the cycle stability of the catalyst under the optimal reaction conditions was further evaluated.The results showed that 2CoP-TiO_(2)prepared with m(NaH_(2)PO_(2))∶m(Co-TiO_(2))=2∶1 exhibited the best catalytic performance.Under the condition of visible light irradiation,reaction temperature 298 K,2CoP-TiO_(2)20 mg,AB aqueous solution 60 mL with a concentration of 0.5 mol/L,the conversion frequency of the reaction reached the highest of 38.7 min^(-1),with an activation energy of 46.4 kJ/mol.The 2CoP-TiO_(2)also displayed good cycle stability.After 5 cycles of testing,the reaction time did not increase significantly.The introduction of phosphorus reduced the band gap energy from 2.70 eV of Co-TiO_(2)to 2.46 eV of 2CoP-TiO_(2),which improved the electron migration rate and promoted the photocatalytic reaction.
作者
许立信
康梦奇
周洋
谢婧
郝思雨
万超
XU Lixin;KANG Mengqi;ZHOU Yang;XIE Jing;HAO Siyu;WAN Chao(School of Chemistry and Chemical Engineering,Anhui University of Technology,Ma'anshan 243032,Anhui,China;Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University,Tianjin 300071,China;Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,Changzhou University,Changzhou 213164,Jiangsu,China;College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310058,Zhejiang,China)
出处
《精细化工》
北大核心
2025年第9期2014-2021,共8页
Fine Chemicals
基金
国家自然科学基金青年基金项目(22108238)、面上基金项目(22478001)和联合项目(U22A20408)
安徽省自然科学基金青年基金项目(1908085QB68)
中国博士后面上项目(2019M662060)
派出项目(PC2022046)
特别资助项目(2020T130580)
江苏省绿色催化材料与技术重点实验室项目(BM2012110)
2022、2023年国家级大学生创新创业训练计划项目(202210360037、S202310260212)
生物膜法水质净化及利用技术教育部工程研究中心开放基金资助项目(BWPU2023KF06)
安徽省高校优秀青年科研项目(2024AH030008)
安徽省科技厅优秀青年基金项目(2408085Y005)
关键词
磷化钴
二氧化钛
氨硼烷
水解制氢
光催化
cobalt phosphide
titanium dioxide
ammonia borane
hydrogen hydrolysis
photocatalysis
