Surface-mediated selective photocatalytic aerobic oxidation reactions on TiO2 nanofibres
Surface-mediated selective photocatalytic aerobic oxidation reactions on TiO2 nanofibres
复制标题
TiO2 纳米纤维表面介导的选择性光催化有氧氧化反应
DOI：
10.1039/c5ra07518a
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发表时间：
2015-06
期刊：
影响因子：
3.9
通讯作者：
Zheng Zhanfeng
中科院分区：
文献类型：
--
作者：
Huang Lizhi;Jia Jianfeng;Liu Hongwei;Yuan Yong;Zhao Jian;Chen Shuai;Fan Weibin;Waclawik Eric R.;Zhu Huaiyong;Zheng Zhanfeng
N掺杂的TiO 2纳米纤维具有较低的好氧氧化活性比未掺杂的TiO 2纳米纤维在选择性光催化好氧氧化苄胺和4-甲氧基苯甲醇。这是由于减少自由能的O2吸附在附近的氮掺杂剂的网站，所示的密度泛函理论（DFT）计算时，三配位的氧原子被氮原子取代。发现在空气中受控煅烧N掺杂NF后活性恢复。苄胺和4-甲氧基苄醇的转化率对光照强度的依赖性证实了这些反应是由光驱动的。作用光谱表明，这两个氧化反应响应的光从紫外区到可见光照射范围。扩展的光吸收波长范围在这些系统中相比，纯TiO 2材料被发现从形成的表面络合物物种的反应物吸附到催化剂的表面上，证明了原位IR实验。催化氧化和原位红外光谱分析结果表明，苯甲醛是苄胺有氧氧化合成N-亚苄基苄胺的中间体。
N-doped TiO2 nanofibres were observed to possess lower aerobic oxidation activity than undoped TiO2 nanofibres in the selective photocatalytic aerobic oxidation of benzylamine and 4-methoxybenzyl alcohol. This was attributed to the reduction free energy of O2 adsorption in the vicinity of nitrogen dopant sites, as indicated by density functional theory (DFT) calculations when three-coordinated oxygen atoms are substituted by nitrogen atoms. It was found that the activity recovered following a controlled calcination of the N-doped NFs in air. The dependence of the conversion of benzylamine and 4-methoxybenzyl alcohol on the intensity of light irradiation confirmed that these reactions were driven by light. Action spectra showed that the two oxidation reactions are responsive to light from the UV region through to the visible light irradiation range. The extended light absorption wavelength range in these systems compared to pure TiO2 materials was found to result from the formation of surface complex species following adsorption of reactants onto the catalysts' surface, evidenced by the in situ IR experiment. Both catalytic and in situ IR results reveal that benzaldehyde is the intermediate in the aerobic oxidation of benzylamine to N-benzylidenebenzylamine process.
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影响因子：
17.1
作者：
Hongwei Liu;Zhanfeng Zheng;Dongjiang Yang;Xuebin Ke;E. Jaatinen;Jin-cai Zhao;Huaiyong Zhu
通讯作者：
Hongwei Liu;Zhanfeng Zheng;Dongjiang Yang;Xuebin Ke;E. Jaatinen;Jin-cai Zhao;Huaiyong Zhu
影响因子：
22.1
作者：
Kobayashi, Hisayoshi;Higashimoto, Shinya
通讯作者：
Higashimoto, Shinya
影响因子：
7.4
作者：
Hawkins, CL;Davies, MJ
通讯作者：
Davies, MJ
影响因子：
--
作者：
Bakardjieva, S;Stengl, V;Petrova, N
通讯作者：
Petrova, N
影响因子：
3.3
作者：
Diwald, O;Thompson, TL;Yates, JT
通讯作者：
Yates, JT