Selective chemical looping combustion of acetylene in ethylene-rich streams

IF 45.8 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Science Pub Date : 2025-02-13
Matthew Jacob, Huy Nguyen, Rishi Raj, Javier Garcia-Barriocanal, Jiyun Hong, Jorge E. Perez-Aguilar, Adam S. Hoffman, K. Andre Mkhoyan, Simon R. Bare, Matthew Neurock, Aditya Bhan
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Abstract

The requirement for C2H2 concentrations below 2 parts per million (ppm) in gas streams for C2H4 polymerization necessitates its semihydrogenation to C2H4. We demonstrate selective chemical looping combustion of C2H2 in C2H4-rich streams by Bi2O3 as an alternative catalytic pathway to reduce C2H2 concentration below 2 ppm. Bi2O3 combusts C2H2 with a first-order rate constant that is 3000 times greater than the rate constant for C2H4 combustion. In successive redox cycles, the lattice O of Bi2O3 can be fully replenished without discernible changes in local Bi coordination or C2H2 combustion selectivity. Heterolytic activation of C–H bonds across Bi–O sites and the higher acidity of C2H2 results in lower barriers for C2H2 activation than C2H4, enabling selective catalytic hydrocarbon combustion leveraging differences in molecular deprotonation energies.
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富乙烯流中乙炔的选择性化学环燃烧
C2H4聚合要求气体流中的C2H2浓度低于百万分之2 (ppm),因此需要将其半加氢成C2H4。我们证明了Bi2O3在富C2H2流中选择性化学环燃烧C2H2作为一种替代催化途径,将C2H2浓度降低到2 ppm以下。Bi2O3燃烧C2H2的一级速率常数是C2H4燃烧速率常数的3000倍。在连续的氧化还原循环中,Bi2O3的晶格O可以得到充分补充,而局部Bi配位和C2H2燃烧选择性没有明显的变化。跨Bi-O位点的C-H键的异裂解活化和C2H2较高的酸性导致C2H2的活化障碍比C2H4低,从而利用分子去质子化能的差异实现选择性催化烃类燃烧。
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来源期刊
Science
Science 综合性期刊-综合性期刊
CiteScore
61.10
自引率
0.90%
发文量
0
审稿时长
2.1 months
期刊介绍: Science is a leading outlet for scientific news, commentary, and cutting-edge research. Through its print and online incarnations, Science reaches an estimated worldwide readership of more than one million. Science’s authorship is global too, and its articles consistently rank among the world's most cited research. Science serves as a forum for discussion of important issues related to the advancement of science by publishing material on which a consensus has been reached as well as including the presentation of minority or conflicting points of view. Accordingly, all articles published in Science—including editorials, news and comment, and book reviews—are signed and reflect the individual views of the authors and not official points of view adopted by AAAS or the institutions with which the authors are affiliated. Science seeks to publish those papers that are most influential in their fields or across fields and that will significantly advance scientific understanding. Selected papers should present novel and broadly important data, syntheses, or concepts. They should merit recognition by the wider scientific community and general public provided by publication in Science, beyond that provided by specialty journals. Science welcomes submissions from all fields of science and from any source. The editors are committed to the prompt evaluation and publication of submitted papers while upholding high standards that support reproducibility of published research. Science is published weekly; selected papers are published online ahead of print.
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