Bimetallic oxide catalysis meets silanol-enhanced synergy: A winning combination for efficient CO2 fixation by cycloaddition with styrene oxide

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-03-22 DOI:10.1016/j.mcat.2025.115029
Chaitra N. Mallannavar , S. Sujith , Shrinidhi D. Patil , Sanjeev P. Maradur , Ganapati V. Shanbhag
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Abstract

The bimetallic oxide dispersed on silanol rich SBA-15-OH was designed for the synthesis of cyclic carbonates from epoxides and CO2. The SBA-15-OH was synthesized via desilication and active metals were loaded by sol-gel method. Pure Sn-Ni oxide with a low surface area and lesser activity was modified by dispersing it on a high surface area SBA-15-OH. The different characterization techniques such as XRD, N2-sorption, CO2 and NH3-TPD, H2-TPR, SEM-EDX, TEM and XPS confirmed that the surface silanol group acts as anchoring site for the enhanced metal oxide-support interaction. Supported Sn-Ni oxide exhibited 16-fold better activity than pure Sn-Ni oxide, due to improved dispersion, which enhances the accessibility of reactants to the catalytic sites. Under the optimized reaction conditions 10Sn5Ni/SBA-15-OH gave 92.9 % styrene oxide conversion and 84.3 % selectivity for styrene carbonate. The catalyst is recyclable and the flexibility of the catalyst is tested for different epoxides with CO2.

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双金属氧化物催化满足硅醇增强的协同作用:通过环加成与苯乙烯氧化物有效的CO2固定的成功组合
设计了分散在富含硅醇的SBA-15-OH上的双金属氧化物,用于环氧化物和CO2合成环状碳酸盐。采用脱硅法制备SBA-15-OH,并采用溶胶-凝胶法负载活性金属。将低表面积、低活性的纯Sn-Ni氧化物分散在高表面积的SBA-15-OH上进行改性。通过XRD、n2吸附、CO2和NH3-TPD、H2-TPR、SEM-EDX、TEM和XPS等表征手段证实,表面硅醇基是金属氧化物-载体相互作用增强的锚定位点。负载型Sn-Ni氧化物表现出比纯Sn-Ni氧化物高16倍的活性,这是由于分散性的改善,提高了反应物对催化位点的接近性。在优化的反应条件下,10Sn5Ni/SBA-15-OH对苯乙烯的氧化转化率为92.9%,对苯乙烯的选择性为84.3%。催化剂是可回收的,催化剂的柔韧性测试了不同的环氧化物与二氧化碳。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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