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Zn2+ stabilized Pd clusters with enhanced covalent metal-support interaction via the formation of Pd-Zn bonds to promote catalytic thermal stability.
Nanoscale ( IF 5.8 ) Pub Date : 2020-06-24 , DOI: 10.1039/d0nr02987d Kai-Qiang Jing 1 , Yu-Qing Fu 1 , Zhi-Qiao Wang 2 , Zhe-Ning Chen 2 , Hong-Zi Tan 2 , Jing Sun 2 , Zhong-Ning Xu 2 , Guo-Cong Guo 2
Nanoscale ( IF 5.8 ) Pub Date : 2020-06-24 , DOI: 10.1039/d0nr02987d Kai-Qiang Jing 1 , Yu-Qing Fu 1 , Zhi-Qiao Wang 2 , Zhe-Ning Chen 2 , Hong-Zi Tan 2 , Jing Sun 2 , Zhong-Ning Xu 2 , Guo-Cong Guo 2
Affiliation
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Pd-Based heterogeneous catalysts have been demonstrated to be efficient in numerous heterogeneous reactions. However, the effect of the support resulting in covalent metal–support interaction (CMSI) has not been researched sufficiently. In this work, a Lewis base is modulated over MgAl-LDH to investigate the support effects and it is further loaded with Pd clusters to research the metal–support interactions. MgAl-LDH with ultra-low Pd loading (0.0779%) shows CO conversion (55.0%) and dimethyl oxalate (DMO) selectivity (93.7%) for CO oxidative coupling to DMO, which was gradually deactivated after evaluation for 20 h. To promote the stability of Pd/MgAl-LDH, Zn2+ ions were introduced into the MgAl-LDH support to strengthen the CMSI by forming Pd–Zn bonds, which further increased the adsorption energy of the Pd clusters on ZnMgAl-LDH, and this was verified by X-ray absorption fine structure (XAFS) measurements and density functional theory (DFT) calculations. The stability of the Pd/ZnMgAl-LDH catalyst could be maintained for at least 100 h. This work highlights that covalent metal–support interactions can be strengthened by forming new metal–metal bonds, which could be extended to other systems for the stabilization of noble metals over supports.
中文翻译：
Zn2 +稳定的Pd簇通过形成Pd-Zn键增强共价金属-载体相互作用，从而促进催化热稳定性。
钯基非均相催化剂已被证明在许多非均相反应中是有效的。但是，尚未充分研究支持物导致共价金属与支持物相互作用（CMSI）的作用。在这项工作中，路易斯碱在MgAl-LDH上进行调制以研究支持作用，并进一步加载Pd团簇以研究金属与支持物的相互作用。具有超低Pd负载量（0.0779％）的MgAl-LDH显示出CO转化率（55.0％）和草酸二甲酯（DMO）对CO氧化成DMO的选择性（93.7％），在评估20小时后逐渐失活。为了提高Pd / MgAl-LDH的稳定性，Zn 2+通过形成Pd-Zn键将离子引入MgAl-LDH载体中以增强CMSI，这进一步增加了ZnMgAl-LDH上Pd团簇的吸附能，这通过X射线吸收精细结构（XAFS）测量得到验证和密度泛函理论（DFT）计算。Pd / ZnMgAl-LDH催化剂的稳定性可以维持至少100小时。这项工作着重指出，可以通过形成新的金属-金属键来增强共价金属与载体之间的相互作用，可以将其扩展到其他系统上，以使贵金属稳定在载体上。
更新日期：2020-07-16
中文翻译：
Zn2 +稳定的Pd簇通过形成Pd-Zn键增强共价金属-载体相互作用，从而促进催化热稳定性。
钯基非均相催化剂已被证明在许多非均相反应中是有效的。但是，尚未充分研究支持物导致共价金属与支持物相互作用（CMSI）的作用。在这项工作中，路易斯碱在MgAl-LDH上进行调制以研究支持作用，并进一步加载Pd团簇以研究金属与支持物的相互作用。具有超低Pd负载量（0.0779％）的MgAl-LDH显示出CO转化率（55.0％）和草酸二甲酯（DMO）对CO氧化成DMO的选择性（93.7％），在评估20小时后逐渐失活。为了提高Pd / MgAl-LDH的稳定性，Zn 2+通过形成Pd-Zn键将离子引入MgAl-LDH载体中以增强CMSI，这进一步增加了ZnMgAl-LDH上Pd团簇的吸附能，这通过X射线吸收精细结构（XAFS）测量得到验证和密度泛函理论（DFT）计算。Pd / ZnMgAl-LDH催化剂的稳定性可以维持至少100小时。这项工作着重指出，可以通过形成新的金属-金属键来增强共价金属与载体之间的相互作用，可以将其扩展到其他系统上，以使贵金属稳定在载体上。
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