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能够实现双极膜中快速水离解的屏蔽型针铁矿催化剂。

Shielded goethite catalyst that enables fast water dissociation in bipolar membranes.

作者信息

Shehzad Muhammad A, Yasmin Aqsa, Ge Xiaolin, Ge Zijuan, Zhang Kaiyu, Liang Xian, Zhang Jianjun, Li Geng, Xiao Xinle, Jiang Bin, Wu Liang, Xu Tongwen

机构信息

CAS Key Laboratory of Soft Matter Chemistry, Collaborative Innovation Centre of Chemistry for Energy Materials, Department of Applied Chemistry, School of Chemistry and Materials Science, University of Science and Technology of China, 230026, Hefei, China.

Advanced Materials and Membranes Technology Centre, Department of Polymer and Process Engineering, University of Engineering and Technology Lahore, G.T. Road, Punjab, 54890, Pakistan.

出版信息

Nat Commun. 2021 Jan 4;12(1):9. doi: 10.1038/s41467-020-20131-1.

DOI:10.1038/s41467-020-20131-1
PMID:33397931
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7782813/
Abstract

Optimal pH conditions for efficient artificial photosynthesis, hydrogen/oxygen evolution reactions, and photoreduction of carbon dioxide are now successfully achievable with catalytic bipolar membranes-integrated water dissociation and in-situ acid-base generations. However, inefficiency and instability are severe issues in state-of-the-art membranes, which need to urgently resolve with systematic membrane designs and innovative, inexpensive junctional catalysts. Here we show a shielding and in-situ formation strategy of fully-interconnected earth-abundant goethite FeO(OH) catalyst, which lowers the activation energy barrier from 5.15 to 1.06 eV per HO - H bond and fabricates energy-efficient, cost-effective, and durable shielded catalytic bipolar membranes. Small water dissociation voltages at limiting current density (U: 0.8 V) and 100 mA cm (U: 1.1 V), outstanding cyclic stability at 637 mA cm, long-time electro-stability, and fast acid-base generations (HSO: 3.9 ± 0.19 and NaOH: 4.4 ± 0.21 M m min at 100 mA cm) infer confident potential use of the novel bipolar membranes in emerging sustainable technologies.

摘要

通过催化双极膜集成水电离和原位酸碱生成,现在已成功实现了高效人工光合作用、析氢/析氧反应以及二氧化碳光还原的最佳pH条件。然而,效率低下和稳定性差是现有技术膜中存在的严重问题,需要通过系统的膜设计以及创新的廉价连接催化剂来紧急解决。在此,我们展示了一种完全互连的富含地球元素的针铁矿FeO(OH)催化剂的屏蔽和原位形成策略,该策略将每个HO-H键的活化能垒从5.15 eV降低至1.06 eV,并制造出了节能、经济高效且耐用的屏蔽催化双极膜。在极限电流密度(U:0.8 V)和100 mA cm(U:1.1 V)下的小水电离电压、在637 mA cm下出色的循环稳定性、长期电稳定性以及快速的酸碱生成(在100 mA cm下,HSO:3.9±0.19和NaOH:4.4±0.21 M m min)表明,这种新型双极膜在新兴可持续技术中具有可靠的潜在应用价值。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/d87fdba9833b/41467_2020_20131_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/8c88fe219798/41467_2020_20131_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/d6bbf98bd638/41467_2020_20131_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/80ea72b510fb/41467_2020_20131_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/608320ec5e25/41467_2020_20131_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/e949b3a32a19/41467_2020_20131_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/d87fdba9833b/41467_2020_20131_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/8c88fe219798/41467_2020_20131_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/d6bbf98bd638/41467_2020_20131_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/80ea72b510fb/41467_2020_20131_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/608320ec5e25/41467_2020_20131_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/e949b3a32a19/41467_2020_20131_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9939/7782813/d87fdba9833b/41467_2020_20131_Fig6_HTML.jpg

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