Citation: Zengtian Chen, Yuxue Xiao, Chao Zhang, Zaihui Fu, Ting Huang, Qingfeng Li, Yuanxiong Yao, Shutao Xu, Xiaoli Pan, Wenhao Luo, Changzhi Li. Fabrication of a solid superacid with temperature-regulated silica-isolated biochar nanosheets[J]. Chinese Journal of Catalysis, ;2020, 41(4): 698-709. doi: S1872-2067(19)63522-9 shu

Fabrication of a solid superacid with temperature-regulated silica-isolated biochar nanosheets

Zengtian Chen ^a,b, ,
Yuxue Xiao ^a,b ,
Chao Zhang ^a ,
Zaihui Fu ^a ,
Ting Huang ^a ,
Qingfeng Li ^a ,
Yuanxiong Yao ^a ,
Shutao Xu ^b ,
Xiaoli Pan ^b ,
Wenhao Luo ^b ,
Changzhi Li ^b,c

a National & Local Joint Engineering Laboratory for New Petro-chemical Materials and Fine Utilization of Resources and Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research (Ministry of Education), College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha 410081, Hunan, China;
b Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
c Dalian National Laboratory for Clean Energy, Chinese Aacdemy of Sciences, Dalian 116023, Liaoning, China

Received Date: 26 October 2019
Revised Date: 23 November 2019

Fund Project: We acknowledge the financial support for this work by the National Natural Science Foundation of China (21690080, 21676079, 21546010, 21690083, 21878288), the Strategic Priority Research Program of Chinese Academy of Sciences (XDB17020100), the Natural Science Foundation of Hunan Province (2018JJ3335), the Innovation Platform Open Fund of Hunan College (18K016), and DNL Cooperation Fund CAS (DNL180302).

This paper reports a new strategy for the structural reconstruction of biomass carbon sulfonic acid (BCSA) to its solid superacid counterpart. In this approach, a cheap layered biomass carbon (BC) source is chemically exfoliated by cetyltrimethyl ammonium bromide and then converted to silica-isolated carbon nanosheets (CNSs) by a series of conversion steps. The state of the silica-isolated CNSs and the stacking density of their nanoparticles are regulated by the dehydration temperature. Only the highly isolated and non-crosslinked CNSs with loose particle stacking structures obtained upon dehydration at 250℃ can be turned into superacid sites (with stronger acidity than that of 100% H₂SO₄) after sulfonation. This is accompanied by the creation of abundant hierarchical slit pores with high external surface area, mainly driven by the strong hydrogen bonding interactions between the introduced sulfonic acid groups. In typical acid-catalyzed esterification, etherification, and hydrolysis reactions, the newly formed superacid exhibits superior catalytic activity and stability compared to those of common BCSA and commercial Amberlyst-15 catalysts, owing to its good structural stability, highly exposed stable superacidic sites, and abundance of mesoporous/macroporous channels with excellent mass transfer rate. This groundbreaking work not only provides a novel strategy for fabricating bio-based solid superacids, but also overcomes the drawbacks of BCSA, i.e., unsatisfactory structural stability, acidity, and porosity.
- Biomass conversion,
- Bio-based sulfonic acid,
- Silica isolation,
- Solid superacid,
- Acid catalysis
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