In situ MnOx/N-doped carbon aerogels from cellulose as monolithic and highly efficient catalysts for the upgrading of bioderived aldehydes,Green Chemistry

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In situ MnOx/N-doped carbon aerogels from cellulose as monolithic and highly efficient catalysts for the upgrading of bioderived aldehydes
Green Chemistry ( IF 9.3 ) Pub Date : 2018-06-29 , DOI: 10.1039/c8gc01413b
Shenghui Zhou _{1,

2,

3,

4} , Guixian Chen _{1,

2,

3,

4} , Xiao Feng _{1,

2,

3,

4} , Ming Wang _{1,

2,

3,

4} , Tao Song _{1,

2,

3,

4} , Detao Liu _{1,

2,

3,

4} , Fachuang Lu _{1,

2,

3,

4,

5} , Haisong Qi _{1,

2,

3,

4,

5}

Affiliation

Herein, we report a sustainable route to in situ synthesize a monolithic MnO_x/N-doped carbon aerogel catalyst (Mn-NCA) by pyrolysing MnO(OH)₂-cellulose aerogel precursors based on an alkali–urea aqueous system. The as-obtained Mn-NCA showed highly efficient catalytic activity for the transfer hydrogenation of a broad range of biomass-derived aldehydes, yielding 90–100% conversion and 64–100% selectivity to the corresponding alcohols under mild conditions in an oven without agitation. A combination of controlled experiments and detailed characterization studies indicated that the superior performance of Mn-NCA is attributed to the monolithic three-dimensional (3D) hierarchical porous architecture and the synergistic effects between homogeneously dispersed MnO_x nanoparticles (NPs) and urea-derived basic sites. The monolithic feature of Mn-NCA exhibits superior dispersibility and separability compared to conventional centrifugation and filtration techniques in a powdery catalytic system. Moreover, a possible reaction mechanism is proposed. Our work provides a new method for developing highly efficient monolithic catalysts from renewable biopolymers for biomass valorization.

中文翻译：

来自纤维素的原位MnO _x / N掺杂碳气凝胶，作为整体和高效催化剂，用于生物衍生醛的提质

在本文中，我们报告了一种通过在碱-尿素水体系基础上热解MnO（OH）_2-纤维素气凝胶前体来原位合成整体式MnO _x / N掺杂碳气凝胶催化剂（Mn-NCA）的可持续途径。所获得的Mn-NCA对多种生物质衍生的醛的转移加氢显示出高效的催化活性，在温和的条件下，在无搅拌的烘箱中，可获得90-100％的转化率和对相应醇的64-100％的选择性。。对照实验和详细表征研究的结合表明Mn-NCA的优异性能归因于整体式三维（3D）分层多孔结构以及均匀分散的MnO之间的协同效应_x纳米颗粒（NPs）和尿素衍生的碱性位点。与传统的粉状催化系统中的离心和过滤技术相比，Mn-NCA的整体特征具有优异的分散性和可分离性。此外，提出了可能的反应机理。我们的工作为从可再生生物聚合物开发高效整体式催化剂提供了一种新方法，以用于生物质增值。

更新日期：2018-07-30

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