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Fe3+-Mediated Pt/Y Zeolite Catalysts Display Enhanced Metal–Bronsted Acid Interaction and Synergistic Cascade Hydrogenolysis Reactions
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-07-12 , DOI: 10.1021/acs.iecr.0c01971
Guangyu Zhang 1 , Xin Jin 1 , Jinyao Wang 1 , Mengyuan Liu 1 , Wenxiang Zhang 1 , Yujie Gao 1 , Xiaoqing Luo 1 , Qinqin Zhang 2 , Jian Shen 3 , Chaohe Yang 1
Affiliation  

Strong metal–Bronsted acid interaction is critical for interfacial catalysis. Tunable electronic coupling at the metal/acid interface for tandem C–H and C–O bond activation has been largely unexplored. We reported a simple design principle for Pt–Fe3+ interfacial catalysts to tailor the electron structure between metallic and structural acidic frameworks via the strong Pt-Bronsted acid interaction, for cascade hydrogenolysis of glycerol involving tandem C–H and C–O cleavage. One of the key findings in this work is that the formation of Fe(OH)O species in Pt–Fe3+ hybrids contributes to the enhanced surface Bronsted acidity and weakened Pt–H binding strength. Thus, the proposed Pt-Bronsted acid catalysts show synergistic performances for cascade hydrogenolysis of glycerol, with a 3-fold activity (turnover frequency (TOF) = 455.2 h–1) and enhanced selectivity toward ethylene glycol and propylene glycol (combined selectivity of ∼70%), compared to monometallic Pt/Y-IM catalysts (TOF = 106.3 h–1, selectivity = 16.2%). In addition, the size-sensitivity studies on Pt–Fe3+ catalysts with Pt particle sizes ranging from 1.8 nm to 3.8 nm showed that catalytic C–H and C–O bond cleavage possibly follow σ- and π-bond activation mechanisms, respectively. The simple strategy discussed in this work for synthesizing metal–acid catalysts provides new insights into rational design of effective catalysts for cascade hydrogenolysis of various other bioderived oxygenates to value-added products.

中文翻译:

Fe 3+介导的Pt / Y沸石催化剂显示出增强的金属-布朗斯台德酸相互作用和协同级联氢解反应

金属与布朗斯台德酸之间的强相互作用对于界面催化至关重要。串联C–H和C–O键活化的金属/酸界面上的可调电子耦合在很大程度上尚未得到开发。我们报道了一种简单的Pt-Fe 3+界面催化剂的设计原理,可以通过强Pt-布朗斯台德酸相互作用来调节金属和结构酸性构架之间的电子结构,从而实现涉及C-H和C-O裂解的甘油的级联氢解。这项工作的主要发现之一是在Pt–Fe 3+中形成了Fe(OH)O物种。杂种有助于增强表面布朗斯台德酸度和减弱Pt–H结合强度。因此,拟议的Pt-布朗斯台德酸催化剂显示出甘油级联氢解的协同性能,具有3倍的活性(转换频率(TOF)= 455.2 h –1),并且对乙二醇和丙二醇的选择性提高(组合选择性为〜与单金属Pt / Y-IM催化剂(TOF = 106.3 h –1,选择性= 16.2%)相比,降低了70%。此外,对Pt–Fe 3+的尺寸敏感性研究Pt粒径在1.8 nm至3.8 nm范围内的催化剂表明,催化的C–H和C–O键裂解可能分别遵循σ和π键活化机理。这项工作中讨论的用于合成金属酸催化剂的简单策略为合理设计合理的催化剂提供了新的见解,该催化剂可用于将各种其他生物衍生的含氧化合物级联氢解为增值产品。
更新日期:2020-07-12
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