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高分子修饰Pt/ZnS-CdS/SiO2催化剂表面官能团调变与光催化制氢活性关系的研究
  • ISSN号:1001-3555
  • 期刊名称:《分子催化》
  • 时间:0
  • 分类:O643.32[理学—物理化学;理学—化学]
  • 作者机构:[1]兰州大学化学与化工学院,甘肃兰州730000, [2]中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室,甘肃兰州730000, [3]中国航天医学工程研究所,北京100094
  • 相关基金:2007CB613305,2009CB22003,和2009AA05Z117,21173242中科院太阳能行动计划KGCX2-YW-390-1和KGCV2-YW-390-3资助
中文摘要:

用丙烯酸酯和环氧树脂将亲水性的-OH和芳香性的苯环修饰到Pt/ZnS-CdS/SiO2催化剂表面,在不同气氛下进行热处理,得到了表面修饰并热处理后的Pt/ZnS-CdS/SiO2光催化剂,考察催化剂的可见光催化分解水产氢活性.结果表明修饰并热处理后催化剂活性不同程度的下降.XRD结果表明,修饰前后ZnS和CdS的特征衍射峰没有改变,但空气热处理致使催化剂晶型由立方晶型的CdS和六方晶型的ZnS向六方晶型的CdS和α-ZnS的转变,氢气气氛热处理致使催化剂的晶型向六方结构的固溶体Zn0.5Cd0.5S转变,未修饰的催化剂在空气和氢气中热处理后晶型发生了同样的转变.HRTEM结果表明表面修饰后催化剂平均粒径由18 nm减小为6 nm,仍以ZnS为外层,CdS为内层的核壳结构形态存在.紫外可见漫反射(UV-Vis DRS)结果表明,经修饰和热处理后的光催化剂在450~800 nm区间的光吸收增加,在空气中773 K煅烧后的催化剂的吸收限由480 nm红移至520 nm,而在氢气中于773 K煅烧后吸收限则由480 nm蓝移至420 nm.修饰后催化剂的羟基吸收强度增大,出现了苯环的特征吸收峰,这些官能团经热处理后发生了显著变化.红外光谱(IR)结果表明空气热处理导致部分含氧官能团发生了脱离,羟基吸收增强;氢气热处理导致C—O和C—O—C的吸收峰增强,同时催化剂表面发生碳化.热重差热分析(TG-DTA)与红外结果均证实了这种变化.产氢活性下降可能归结为表面羟基减少导致的在反应体系中的分散性和光生电荷的分离效率降低;催化剂表面的含氧官能团占据了催化活性位并且降低了颗粒在水溶液中的分散性.

英文摘要:

The hydrophilic-OH group and aromatic benzene ring were modified to the surface of Pt/ZnS-CdS/SiO2 photocatalyst using acrylate and epoxy resin.Then the particles were calcined in the atmosphere and in the hydrogen at different temperatures.The photocatalytic hydrogen-producing activities of the obtained photocatalysts were investigated.The results showed that modification and heat treatment resulted in activity decrease by different degrees.The XRD results showed that the characteristic peaks of ZnS and CdS were not changed after modification,but the change from cubic-type CdS and hexagonal-type ZnS into hexagonal-type CdS and α-ZnS after heat treatment in the air were observed.In addition,the hexagonal structure solid solution Zn0.5Cd0.5S was formed during hydrogen treatment.The heat treatment of unmodified catalysts both in the air and in the hydrogen led to the same phase transformation.HRTEM results showed that the catalyst's average diameter reduced from 18 nm to 6 nm after surface modification,while the structure of a CdS core and ZnS shell in photocatalyst was remained.UV-Vis DRS results showed that the light absorption of the photocatalysts were enhanced after modification and heat treatment in the range of 450 to 800 nm.The absorption edge of the catalyst red shifted from 480 nm to 520 nm after heat treatment at 773 K in the air,while it blue shifted from 480 nm to 420 nm after treatment in the hydrogen.The hydroxyl absorption was enhanced after modification,and the characteristic absorption of benzene ring appeared.IR results showed that these functional groups had significant changed after heat treatment.Some hydroxyl absorption was enhanced when the catalyst was underwent heat treatment in the air,while the absorption of C-O and C-O-C were enhanced in the hydrogen.These changes were also confirmed by TG-DTA results.The decrease of hydrogen-producing activity may be attributed to the decrease of catalyst's dispersion and the decrease of separation efficiency of photogenerated charges,both of whic

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期刊信息
  • 《分子催化》
  • 中国科技核心期刊
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院兰州化学物理研究所
  • 主编:李树本
  • 地址:兰州市天水路18号
  • 邮编:730000
  • 邮箱:fzch@licp.cas.cn
  • 电话:0931-4968226
  • 国际标准刊号:ISSN:1001-3555
  • 国内统一刊号:ISSN:62-1039/O6
  • 邮发代号:54-69
  • 获奖情况:
  • 1992年获中国科学院优秀期刊三等奖,1992年获甘肃省第二届优秀科技期刊荣誉称号
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),中国北大核心期刊(2000版)
  • 被引量:7932