CO2 Hydrogenation to Formate by Palladium Nanoparticles Supported on N-Incorporated Periodic Mesoporous Organosilica,ACS Sustainable Chemistry & Engineering

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CO2 Hydrogenation to Formate by Palladium Nanoparticles Supported on N-Incorporated Periodic Mesoporous Organosilica
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-09-04 , DOI: 10.1021/acssuschemeng.0c03860
K. J. Betsy _{1,

2} , Anish Lazar ₁ , Anjuna Pavithran ₁ , C. P. Vinod _{1,

2}

Affiliation

Development of a heterogeneous catalyst capable of selective transformation of CO₂ to valuable products still remains a challenge. In this article, we account for the surfactant-directed synthesis of a new framework-incorporated nitrogen-containing periodic mesoporous organosilica nanosphere (NPMO). A thoroughly characterized N-incorporated hybrid PMO was utilized as a platform for stabilizing well-dispersed and easily accessible Pd nanoparticles (Pd-NPMO) without using any stabilizing agents or expensive dendrimers. Further, this bifunctional hybrid catalyst has been demonstrated to heterogeneously catalyze aqueous phase CO₂ hydrogenation (CO₂/H₂ ratio 1:3) for the direct synthesis of formate under 4 MPa pressure and at 100 °C. To validate the superior performance of the Pd-NPMO catalyst, we compared the activity with Pd-SBA-15 catalysts, and the results showed a 10-fold increase in turnover frequency of 108 h^–1 using Pd on NPMO which envisaged the crucial role of nitrogen sites in this catalyst to boost the CO₂ valorization to formate.

中文翻译：

N结合的周期性介孔有机硅负载的钯纳米颗粒将CO ₂加氢生成甲酸酯

能够选择性地将CO ₂转化为有价值的产物的非均相催化剂的开发仍然是一个挑战。在本文中，我们解释了新的骨架结合的含氮的周期性介孔有机硅纳米球（NPMO）的表面活性剂定向合成。一个经过充分表征的掺氮杂化PMO被用作稳定化分散良好且易于使用的Pd纳米颗粒（Pd-NPMO）的平台，而无需使用任何稳定剂或昂贵的树枝状聚合物。此外，该双功能杂化催化剂已被证明能够异相催化水相CO ₂加氢（CO ₂ / H ₂比例1：3），可在4 MPa压力和100°C下直接合成甲酸。为了验证Pd-NPMO催化剂的优越性能，我们将其活性与Pd-SBA-15催化剂进行了比较，结果表明，在NPMO上使用Pd可以将108 h ^–1的周转频率提高10倍，这是至关重要的在该催化剂中的氮位点的增加以促进CO ₂价位化成甲酸盐。

更新日期：2020-10-05

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