Volume 58, Issue 31 pp. 10671-10676
Communication

Efficient and Selective Methane Borylation Through Pore Size Tuning of Hybrid Porous Organic-Polymer-Based Iridium Catalysts

Dr. Qi Chen

Dr. Qi Chen

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228 P. R. China

These authors contributed equally to this work.

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Anwang Dong

Anwang Dong

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228 P. R. China

These authors contributed equally to this work.

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Dongxu Wang

Dongxu Wang

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228 P. R. China

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Lu Qiu

Lu Qiu

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228 P. R. China

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Dr. Chunxin Ma

Dr. Chunxin Ma

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228 P. R. China

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Dr. Yihui Yuan

Dr. Yihui Yuan

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228 P. R. China

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Prof. Dr. Yunpeng Zhao

Prof. Dr. Yunpeng Zhao

State Key Laboratory of Coastal and Offshore Engineering, Dalian University of Technology, Dalian, 116024 P. R. China

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Prof. Dr. Na Jia

Prof. Dr. Na Jia

Petroleum Systems Engineering, Faculty of Engineering and Applied Science, University of Regina, Regina, Saskatchewan, S4S 0A2 Canada

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Prof. Dr. Zhanhu Guo

Prof. Dr. Zhanhu Guo

Integrated Composites Laboratory (ICL), Department of Chemical & Biomolecular Engineering, University of Tennessee, Knoxville, TN, 37996 USA

College of Chemical and Environmental Engineering, Shandong University of Science and Technology, Qingdao, 266590 P. R. China

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Prof. Dr. Ning Wang

Corresponding Author

Prof. Dr. Ning Wang

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228 P. R. China

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First published: 29 May 2019
Citations: 31

Graphical Abstract

Pore patrol: A series of heterogenous catalysts based on iridium complexes bound inside porous polycarbazoles was prepared for the selective monoborylation of methane. Catalysts with high efficiency and good chemoselectivity can be developed through tuning the pore size distribution of the porous polycarbazole.

Abstract

As a new energy source that could replace petroleum, the global reserves of methane hydrate (combustible ice) are estimated to be approximately 20 000 trillion cubic meters. A large amount of methane hydrate has been found under the seabed, but the transportation and storage of methane gas far from coastlines are technically unfeasible and expensive. The direct conversion of methane into value-added chemicals and liquid fuels is highly desirable but remains challenging. Herein, we prepare a series of iridium complexes based on porous polycarbazoles with high specific areas and good thermochemical stabilities. Through structure tuning we optimized their catalytic activities for the selective monoborylation of methane. One of these catalysts (CAL-3-Ir) can produce methyl boronic acid pinacol ester (CH3Bpin) in 29 % yield in 9 h with a turnover frequency (TOF) of approximately 14 h−1. Because its pore sizes favor monoborylated products, it has a high chemoselectivity for monoborylation (CH3Bpin:CH2(Bpin)2=16:1).

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