In situ capture and value-added utilization of CO2 from flue gas using an ionic liquid polymer supported Zn catalyst†

IF 9.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Green Chemistry Pub Date : 2025-06-24 DOI:10.1039/D5GC02324F
Hongyan Ni, Kang Zhao, Shujuan Liu, Xingchao Dai, Ce Liu, Xionghou Gao, Junyi Zhang, Honghai Liu, Kuo-Wei Huang, Xinjiang Cui and Feng Shi
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Abstract

In this work, a porous organic polymer supported Zn catalyst (Zn@PIP-1) complexed with an ionic liquid (IL), zinc halide (ZnX2), and vinyl-functionalized triphenylphosphine (p-3vPPh3) has been synthesized by a one-pot method and used for the capture and conversion of waste carbon dioxide (CO2 19.4%) from flue gases of complex composition into valuable cyclic carbonates. Combined structure characterization studies of Zn@PIP-1 revealed successful integration of multiple sites and excellent structural stability, conferring high activity and stability under mild, additive-free conditions. The catalyst showed good group tolerance and a series of carbonates with different structures were successfully obtained in high yields. In addition, the catalyst was recyclable and could be successively used 5 times without obvious activity loss. We systematically evaluated the catalyst's robustness through rigorous poisoning resistance assessments against major flue gas contaminants. The experimental data revealed exceptional tolerance thresholds: (1) sustained catalytic efficiency (99% yield retention) under extreme oxidative conditions (O2, 53 333 ppm), (2) unimpaired performance at CO concentrations exceeding 33 333 ppm, and (3) 99% product yield maintained in the presence of 51 233 ppm H2O. This work provides some insights into the design of stable polymer catalysts for efficient CO2 transformation.

Abstract Image

使用离子液体聚合物负载Zn催化剂†从烟气中捕获和增值利用CO2
在这项工作中,通过一锅法合成了一种多孔有机聚合物负载的Zn催化剂(Zn@PIP-1),与离子液体(IL)、卤化锌(ZnX2)和乙烯基功能化的三苯基膦(p-3vPPh3)络合,用于从复杂成分的烟气中捕获和转化废二氧化碳(CO2 19.4%)为有价值的环状碳化物。结合结构表征研究Zn@PIP-1揭示了多个位点的成功整合和优异的结构稳定性,在温和,无添加剂的条件下具有高活性和稳定性。该催化剂具有良好的基团耐受性,并以高收率成功制备了一系列不同结构的碳酸盐。该催化剂具有可回收性,可连续使用5次,无明显活性损失。通过对主要烟气污染物进行严格的抗中毒评估,系统地评估了催化剂的稳健性。实验数据显示了优异的耐受性阈值:(1)在极端氧化条件下(O2, 53 333 ppm)保持催化效率(99%的产率保持),(2)在CO浓度超过33 333 ppm时性能不受影响,(3)在51 233 ppm H2O存在下保持99%的产率。这项工作为设计稳定的聚合物催化剂以实现高效的二氧化碳转化提供了一些见解。
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来源期刊
Green Chemistry
Green Chemistry 化学-化学综合
CiteScore
16.10
自引率
7.10%
发文量
677
审稿时长
1.4 months
期刊介绍: Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.
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