非晶态有机锆聚合物制备及其光催化CO2合成甲醇  

Preparation of amorphous organozirconium polymer and its photocatalytic synthesis of methanol from CO2

作　　者：赵远 贺建雄 姜宏[1] 熊春荣[1] ZHAO Yuan;HE Jianxiong;JIANG Hong;XIONG Chunrong(Skate Key Laboratory of Marine Resource Utilization in South China Sea,Special Glass Key Lab of Hainan Province,Hainan University,Haikou 57022&Hainan,China;AVIC Hainan Special Glass Technology Co.,Ltd.,Chengmai 571900,Hainan,China)

机构地区：[1]海南大学南海海洋资源利用国家重点实验室,海南省特种玻璃实验室,海南海口570228 [2]海南中航特玻科技有限公司,海南澄迈571900

出　　处：《精细化工》2020年第6期1163-1170,共8页Fine Chemicals

基　　金：海南省重大科技计划项目(ZDKJ2017011);海南大学科研平台建设(ZY2019HN09)。

摘　　要：采用溶剂热法在增透的多孔玻璃表面制备负载非晶态有机锆聚合物,通过SEM、XRD、BET、FTIR、UV-Vis、ICP、有机元素分析、荧光光谱(PL)及紫外光电子能谱(UPS)等手段对样品进行了表征。结果表明,非晶态有机锆聚合物(2.64 eV)具有比NH2-Ui O-66(Zr)(2.74 eV)更窄的带隙,复合速率较慢的光生电子-空穴对。在光催化反应器中放入2片负载非晶态有机锆的玻璃(总面积50.4 cm2),在300 W的氙灯照射下催化还原CO2合成甲醇,反应4 h后甲醇的产量为443.0μmol,转换频率(TOF)为8.69 h^-1。当0.1 g NH2-UiO-66(Zr)为催化剂时,甲醇的产量为244.3μmol,TOF仅为0.17 h^-1。非晶态有机锆聚合物的光催化性能明显优于NH2-UiO-66(Zr)粉末,且循环稳定性良好。Glass slide immobilized amorphous organozirconium polymer was fabricated by solvethermal method.The sample was characterized by SEM,XRD,BET,FTIR,UV-Vis,ICP,organic element analysis,fluorescence spectroscopy(PL)and ultraviolet photoelectron spectroscopy(UPS).The results showed amorphous organozirconium polymer had a narrower band-gap width(2.64 e V)than NH2-UiO-66(Zr)powder(2.74 eV).Additionally,amorphous organozirconium exhibited slow recombination rate of photogenerated electron-hole pairs.Two pieces of glass slides loaded with amorphous organozirconium were glued together with a total area of 50.4 cm2 to use in the photocatalytic synthesis of methanol from CO2.The reaction was illuminated under a 300 W Xe lamp for 4 h.The yield of methanol was 443.0μmol,and the corresponding turnover frequency(TOF)was 8.69 h^-1.While 0.1 g NH2-UiO-66(Zr)was used as catalyst under the same reaction conditions,the yield of methanol was 244.3μmol,and the TOF was only 0.17 h^-1.Therefore,the photocatalytic performance of amorphous organozirconium polymer is obviously better than that of NH2-UiO-66(Zr)powder and shows good cyclic stability.

关 键 词：非晶态有机锆 甲醇 光催化 转换频率 CO2 功能材料 

分 类 号：TQ426[化学工程] X701[环境科学与工程—环境工程]