Abstract
In this study, a clew-like ZnO superstructure was synthesized by a copolymer-controlled self-assembly homogeneous precipitation method. Ni was impregnated to the clew-like ZnO superstructure to obtain Ni/ZnO adsorbents. The synthesized materials were characterized by scanning electron microscopy, transmission electron microscopy, N2 sorption, X-ray diffraction, Fourier transform infrared spectrometry, and H2-temperature programmed reduction techniques. The reactive adsorption desulfurization (RADS) performance of the adsorbents was evaluated in a fixed bed reactor using thiophene in n-octane as a model fuel. Sample Ni/ZnO-4h exhibits a remarkably high performance with a sulfur capacity of 189.1 mg S g–1, which is above 6 times that of the one prepared with commercial ZnO. Characterization results show that the morphology changes from micro-clews to large solid sticks with the increase of the crystallization time. The loose and open architecture of the clew-like ZnO superstructure facilitates the diffusion of reactants/products, and prevents the adsorbent particles from breakage by supplying space for the volume expansion during the RADS process. The small nanoparticles in ZnO nanostrips result in a high sulfur adsorption capacity and also favor the dispersion of Ni, leading to an excellent RADS performance.
摘要
本文利用共聚物控制均匀沉淀法自组装合成了一种毛线球状ZnO超结构. 通过将Ni浸渍于该氧化锌材料上制备了一系列Ni/ZnO吸 附剂. 其中, 样品Ni/ZnO-4h在反应吸附脱硫中表现出极高的硫容量(189.1 mg S g–1), 是相同条件下使用普通商业ZnO制备的Ni/ZnO-C样 品的6倍. 毛线球状ZnO疏松开放的结构能够促进反应物/产物的扩散, 并抑制体积膨胀对吸附剂结构的破坏. 较小的ZnO颗粒在提供较高 的硫容量的同时还能促进活性组分Ni的分散, 从而导致吸附剂具有较高的反应吸附脱硫性能.
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Acknowledgements
Bai P conceived the idea and arranged the experiments; Liu B conducted the material synthesis and evaluated the adsorbents in RADS; Wu P, Ullah R, Xing W and Yan Z helped in the characterization of materials and data analysis. All authors contributed to the general discussion.
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Peng Bai received his PhD from China University of Petroleum (East China) in 2008. Then, he worked in National University of Singapore as a postdoctoral research fellow. Then he worked in the Institute of Chemical and Engineering Sciences, A*STAR, Singapore, as a scientist. He is currently an associate professor in China University of Petroleum (East China). His research interests focus on the development of porous materials for catalytic applications.
Bowen Liu is currently a master student at the College of Chemical Engineering, China University of Petroleum (East China). His research interest includes nanostructured adsorbents for reactive adsorption desulfurization.
Zifeng Yan received his PhD from Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences in 1994. He is currently the Chair Professor of the State Key Laboratory of Heavy Oil Processing, PetroChina Key Laboratory of Catalysis, and a founding professor of chemical material and catalysis subjects in China University of Petroleum (East China). His research interests focus on the adsorption, catalysis and nanomaterial synthesis and application.
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Bai, P., Liu, B., Wu, P. et al. Remarkably high performance of clew-like ZnO superstructure in reactive adsorption desulfurization. Sci. China Mater. 60, 985–994 (2017). https://doi.org/10.1007/s40843-017-9106-9
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DOI: https://doi.org/10.1007/s40843-017-9106-9