类水滑石Mg3Al1-xFex负载Ir催化剂在肉桂醛加氢反应中的应用:Fe的促进作用

doi:10.1016/S1872-2067(18)63042-6

催化学报 ›› 2018, Vol. 39 ›› Issue (5): 988-996.DOI: 10.1016/S1872-2067(18)63042-6

类水滑石Mg₃Al_1-xFe_x负载Ir催化剂在肉桂醛加氢反应中的应用:Fe的促进作用

林伟伟^a,b, 程海洋^a,b, 李小汝^a,b, 张弨^a,b, 赵凤玉^a,b, 荒井正彦^a,b

a 中国科学院长春应用化学研究所电分析化学国家重点实验室, 吉林长春 130022;
b 中国科学院长春应用化学研究所吉林省绿色化学与过程重点实验室, 吉林长春 130022

收稿日期:2017-12-05 修回日期:2018-02-02 出版日期:2018-05-18 发布日期:2018-04-19
通讯作者: 程海洋
基金资助:
国家重点研发计划（2016YFA0602900）；国家自然科学基金（21603212，21672204）；中国科学院青年创新促进会（2016206）；吉林省科技发展计划（20150204050GX）；中国科学院国际人才计划（2018VCA0012）.

Layered double hydroxide-like Mg₃Al_1-xFe_x materials as supports for Ir catalysts:Promotional effects of Fe doping in selective hydrogenation of cinnamaldehyde

Weiwei Lin^a,b, Haiyang Cheng^a,b, Xiaoru Li^a,b, Chao Zhang^a,b, FengyuZhao^a,b, Masahiko Arai^a,b

a State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China;
b Jilin Province Key Laboratory of Green Chemistry and Process, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China

Received:2017-12-05 Revised:2018-02-02 Online:2018-05-18 Published:2018-04-19
Contact: 10.1016/S1872-2067(18)63042-6
Supported by:
This work was supported by the National Key Research and Development Program of China (2016YFA0602900), National Natural Science Foundation of China (21603212, 21672204), Youth Innovation Promotion Association CAS (2016206), Jilin Provincial Science and Technology Program of China (20150204050GX), and Chinese Academy of Sciences President's International Fellowship Initiative (2018VCA0012).

摘要/Abstract

摘要：

水滑石类化合物（LDH）的层板金属阳离子组成具有可调变性，通过将具有变价特性的过渡金属定量引入LDH层板，经热处理后可以得到具有高比表面积和层板金属原子级分散的混合金属氧化物，后者可广泛用作催化剂载体.如三元Mg-Al-Fe类水滑石材料在光催化、H₂S选择性氧化和乙苯脱氢等反应中表现出较好的活性.Ir催化剂在α，β-不饱和醛加氢反应中具有较好的活性，Fe修饰Ir催化剂可提高不饱和醇选择性，但有关Fe的作用以及Fe与活性组分Ir间的相互作用本质还不是很清楚.
本文以类水滑石材料Mg₃Al_1-xFe_x为载体，采用等体积浸渍法制备了Ir催化剂，并用于肉桂醛加氢反应，通过考察Fe的加入对Ir电子和几何结构的影响揭示了Fe的加入对活性和选择性的影响规律.结果表明，当x从0（Ir/Mg₃Al）增加到1（Ir/Mg₃Fe）时，肉桂醛加氢的反应速率在x=0.25时达到最大值，肉桂醇选择性从44.9%增加到80.3%，且不随肉桂醛转化率的增加而改变.透射电镜结果表明，Ir纳米粒子的粒径随着x的增加未发生明显变化，均为1.7±0.2nm.H₂程序升温还原结果发现Ir可以促进Fe³⁺的还原且两者之间存在相互作用.X射线光电子能谱结果表明，Fe的掺杂没有改变催化剂表面Ir⁰和Ir⁴⁺含量的比值，但当Fe含量增加时，Fe²⁺2p_3/2向高结合能方向偏移，且Ir⁰4f_7/2向低结合能方向偏移，说明电子从Fe²⁺转移到Ir，形成了富电子的Ir物种和缺电子的Fe物种.富电子的Ir物种有利于肉桂醛分子中的C=O键在其表面吸附，并且和Ir相邻的Feⁿ⁺物种可以作为亲电位点吸附肉桂醛分子中氧，从而极化和活化C=O键，因而催化剂活性和选择性增大.采用吸附CO红外光谱表征了催化剂表面的几何结构，2058-2069cm^-1处出现了CO吸附峰，归属于Ir⁰表面CO的线性吸附，高波数2069cm^-1的吸附峰归属于CO在高配位Ir位点（平台）的吸附，低波数2058cm^-1的吸附峰归属于CO在低配位Ir位点（台阶、角、楞）的吸附.随着Fe含量的增加，CO吸附峰蓝移11cm^-1，表明Fe的加入改变了催化剂表面Ir的几何结构，低配位Ir位点减少，高配位Ir位点增多.高配位Ir位点（平台）有利于肉桂醛分子中C=O键的吸附，从而提高了肉桂醇的选择性.总之，Fe的加入虽然没有明显改变Ir纳米粒子的粒径，但却改变了其电子和几何结构，从而提高了催化剂活性和选择性.

关键词: 铱催化剂, 水滑石, 铁掺杂, 载体影响, 选择性加氢, 肉桂醛

Abstract:

Supported Ir catalysts were prepared using layered double hydrotalcite-like materials, such as Mg₃Al_1-xFe_x, containing Fe and Al species in varying amounts as supports. These Ir catalysts were applied for the selective hydrogenation of cinnamaldehyde (CAL). When x was changed from 0 (Ir/Mg₃Al) to 1 (Ir/Mg₃Fe), the rate of CAL hydrogenation reached a maximum at approximately x=0.25, while the selectivity to unsaturated alcohol, i.e., cinnamyl alcohol, monotonously increased from 44.9% to 80.3%. Meanwhile, the size of the supported Ir particles did not change significantly with x, remaining at 1.7 ±0.2 nm, as determined by transmission electron microscopy. The chemical state of Ir and Fe species in the Ir/Mg₃Al_1-xFe_x catalysts was examined by temperature programmed reduction by H₂ and X-ray photoelectron spectroscopy. The surface of the supported Ir particles was also examined through the in-situ diffuse reflectance infrared Fourier-transform of a probe molecule of CO. On the basis of these characterization results, the effects of Fe doping to Mg₃Al on the structural and catalytic properties of Ir particles in selective CAL hydrogenation were discussed. The significant factors are the electron transfer from Fe²⁺ in the Mg₃Al_1-xFe_x support to the dispersed Ir particles and the surface geometry.

Key words: Ir catalyst, Layered double hydroxide, Fe doping, Support effect, Selective hydrogenation, Cinnamaldehyde

林伟伟, 程海洋, 李小汝, 张弨, 赵凤玉, 荒井正彦. 类水滑石Mg₃Al_1-xFe_x负载Ir催化剂在肉桂醛加氢反应中的应用:Fe的促进作用[J]. 催化学报, 2018, 39(5): 988-996.

Weiwei Lin, Haiyang Cheng, Xiaoru Li, Chao Zhang, FengyuZhao, Masahiko Arai. Layered double hydroxide-like Mg₃Al_1-xFe_x materials as supports for Ir catalysts:Promotional effects of Fe doping in selective hydrogenation of cinnamaldehyde[J]. Chinese Journal of Catalysis, 2018, 39(5): 988-996.

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类水滑石Mg₃Al_1-xFe_x负载Ir催化剂在肉桂醛加氢反应中的应用:Fe的促进作用

Layered double hydroxide-like Mg₃Al_1-xFe_x materials as supports for Ir catalysts:Promotional effects of Fe doping in selective hydrogenation of cinnamaldehyde

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