4.8 Article

Assembling covalent organic framework membranes with superior ion exchange capacity

Journal

NATURE COMMUNICATIONS
Volume 13, Issue 1, Pages -

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41467-022-28643-8

Keywords

-

Funding

  1. National Natural Science Foundation of China [21838008, 22008172, U20B2024, 22103054, 21903058]
  2. China Postdoctoral Science Foundation [2020TQ0226, 2021M692384]
  3. Natural Science Foundation of Jiangsu Higher Education Institutions [BK20190810]
  4. Jiangsu Province High-Level Talents [JNHB-106]

Ask authors/readers for more resources

In this study, ionic covalent organic framework membranes (iCOFMs) with high ion exchange capacity were prepared using a dual-activation interfacial polymerization strategy. The reaction at the water-organic interface was accelerated after dual-activation, leading to iCOFMs with high crystallinity and prominent proton conductivity. These covalent organic framework-based membranes are highly tunable and have potential applications in various fields.
Ionic covalent organic framework membranes (iCOFMs) hold great promise in ion conduction-relevant applications because the high content and monodispersed ionic groups could afford superior ion conduction. The key to push the upper limit of ion conductivity is to maximize the ion exchange capacity (IEC). Here, we explore iCOFMs with a superhigh ion exchange capacity of 4.6 mmol g(-1), using a dual-activation interfacial polymerization strategy. Fukui function is employed as a descriptor of monomer reactivity. We use Bronsted acid to activate aldehyde monomers in organic phase and Bronsted base to activate ionic amine monomers in water phase. After the dual-activation, the reaction between aldehyde monomer and amine monomer at the water-organic interface is significantly accelerated, leading to iCOFMs with high crystallinity. The resultant iCOFMs display a prominent proton conductivity up to 0.66 S cm(-1), holding great promise in ion transport and ionic separation applications. Covalent organic framework-based membranes are highly tunable materials with potential use in a variety of applications. Here the authors report a dual-activation interfacial polymerization strategy to prepare ionic covalent organic framework membranes with high ion exchange capacity.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Chemistry, Multidisciplinary

Synergized Cu/Pb Core/Shell Electrocatalyst for High-Efficiency CO2 Reduction to C2+ Liquids

Pengtang Wang, Hao Yang, Yong Xu, Xiaoqing Huang, Juan Wang, Miao Zhong, Tao Cheng, Qi Shao

Summary: The synergistic effect between Cu core and ultrathin Pb shell in Cu/Pb core/shell nanocrystals significantly enhances the electrocatalytic reduction of CO2 toward C2+ liquid products, leading to higher Faradaic efficiency and selectivity. This study highlights the importance of synergistic effect in the design of efficient Cu-based catalysts for CO2 reduction.

ACS NANO (2021)

Article Nanoscience & Nanotechnology

Multiscale Simulation of Solid Electrolyte Interface Formation in Fluorinated Diluted Electrolytes with Lithium Anodes

Peiping Yu, Qintao Sun, Yue Liu, Bingyun Ma, Hao Yang, Miao Xie, Tao Cheng

Summary: The article introduces a fluorinated electrolyte-based lithium metal battery with excellent electrochemical performance. By conducting simulations, it is found that the electrolyte has a good ability to form a solid electrolyte interface (SEI) with a rich LiF layer and polymer layer. These findings provide guidance for the rational design of fluorine-rich electrolytes in the future.

ACS APPLIED MATERIALS & INTERFACES (2022)

Article Nanoscience & Nanotechnology

TiH2 Nanodots Exfoliated via Facile Sonication as Bifunctional Electrocatalysts for Li-S Batteries

Tianran Yan, Yu Wu, Fei Gong, Chen Cheng, Hao Yang, Jing Mao, Kehua Dai, Liang Cheng, Tao Cheng, Liang Zhang

Summary: This study utilizes sonication-assisted liquid-phase exfoliation to fabricate TiH2 nanodots as bifunctional electrocatalysts for lithium-sulfur batteries. The results show that TiH2 nanodots have a strong chemical affinity to polysulfides and can promote the precipitation and decomposition of Li2S, effectively suppressing shuttle effect and improving the redox kinetics of polysulfides.

ACS APPLIED MATERIALS & INTERFACES (2022)

Article Chemistry, Physical

In situ formation of circular and branched oligomers in a localized high concentration electrolyte at the lithium-metal solid electrolyte interphase: a hybrid ab initio and reactive molecular dynamics study

Yue Liu, Qintao Sun, Peiping Yu, Bingyun Ma, Hao Yang, Jiayi Zhang, Miao Xie, Tao Cheng

Summary: Developing advanced electrolytes is crucial for stabilizing the lithium metal anode, with the concept of localized high-concentration electrolyte emerging as an efficient strategy. The underlying reaction mechanism of SEI formation in LHCEs with the Li anode is still unclear, but simulations have provided insights into the basic chemical mechanism of SEI formation.

JOURNAL OF MATERIALS CHEMISTRY A (2022)

Article Multidisciplinary Sciences

Single-site Pt-doped RuO2 hollow nanospheres with interstitial C for high-performance acidic overall water splitting

Juan Wang, Hao Yang, Fan Li, Leigang Li, Jianbo Wu, Shangheng Liu, Tao Cheng, Yong Xu, Qi Shao, Xiaoqing Huang

Summary: In this study, hollow Pt-doped RuO2 nanospheres with interstitial carbon were reported as highly active and stable electrocatalysts for overall water splitting. These catalysts exhibited superior performance compared to most reported catalysts and showed promising stability during continuous operation.

SCIENCE ADVANCES (2022)

Article Multidisciplinary Sciences

Boosting electrocatalytic CO2-to-ethanol production via asymmetric C-C coupling

Pengtang Wang, Hao Yang, Cheng Tang, Yu Wu, Yao Zheng, Tao Cheng, Kenneth Davey, Xiaoqing Huang, Shi-Zhang Qiao

Summary: The authors demonstrate the efficient conversion of CO2 to ethanol using a silver-modified copper-oxide catalyst. By optimizing the coordination number and oxide state of the surface Cu sites, the catalyst accelerates and steers the reaction pathway for ethanol production.

NATURE COMMUNICATIONS (2022)

Article Chemistry, Multidisciplinary

Unveiling the Local Structure and Electronic Properties of PdBi Surface Alloy for Selective Hydrogenation of Propyne

Xuchun Wang, Mingyu Chu, Mengwen Wang, Qixuan Zhong, Jiatang Chen, Zhiqiang Wang, Muhan Cao, Hao Yang, Tao Cheng, Jinxing Chen, Tsun-Kong Sham, Qiao Zhang

Summary: By modulating the surface alloy structure of PdBi, the electronic structure of Pd can be continuously adjusted, leading to enhanced catalytic performance in the selective hydrogenation of propyne.

ACS NANO (2022)

Article Chemistry, Physical

The lattice strain dominated catalytic activity in single-metal nanosheets

Meng Wang, Qintao Sun, Zhenglong Fan, Wenxiang Zhu, Fan Liao, Jie Wu, Yunjie Zhou, Hao Yang, Hui Huang, Mengjie Ma, Tao Cheng, Qi Shao, Mingwang Shao, Zhenhui Kang

Summary: Rational tailoring of nanocatalysts with high efficiency is essential in catalysis research. Strain-engineering offers an effective approach to modulate the electronic structure of electrocatalysts. This study successfully obtained porous flexible iridium nanosheets with tunable compressive strain and established a definite correlation between reactivity and lattice strain.

JOURNAL OF MATERIALS CHEMISTRY A (2023)

Article Chemistry, Multidisciplinary

Programmable Synthesis of High-Entropy Nanoalloys for Efficient Ethanol Oxidation Reaction

Mengfan Li, Chenming Huang, Hao Yang, Yu Wang, Xiangcong Song, Tao Cheng, Jietao Jiang, Yangfan Lu, Maochang Liu, Quan Yuan, Zhizhen Ye, Zheng Hu, Hongwen Huang

Summary: We report a template-directed synthesis method to programmatically fabricate nanoscale high-entropy alloys (HEAs) with controllable compositions and structures by independently controlling the morphology and composition of HEA. A total of 12 nanoscale HEAs with controllable morphologies including zero-dimension nanoparticles, one-dimensional nanowires, two-dimensional ultrathin nanorings (UNRs), and three-dimensional nanodendrites were synthesized. The as-prepared HEA-PdPtCuPbBiUNRs/C showed superior electrocatalytic performance for ethanol oxidation reaction, outperforming commercial Pd/C and Pt/C catalysts in terms of mass activity and durability. This work provides a wide range of nanoscale HEAs and a versatile synthetic strategy with potential impacts in catalysis, sensing, biomedicine, and beyond.

ACS NANO (2023)

Article Multidisciplinary Sciences

Stable and oxidative charged Ru enhance the acidic oxygen evolution reaction activity in two-dimensional ruthenium-iridium oxide

Wenxiang Zhu, Xiangcong Song, Fan Liao, Hui Huang, Qi Shao, Kun Feng, Yunjie Zhou, Mengjie Ma, Jie Wu, Hao Yang, Haiwei Yang, Meng Wang, Jie Shi, Jun Zhong, Tao Cheng, Mingwang Shao, Yang Liu, Zhenhui Kang

Summary: The stability and activity of two-dimensional ruthenium-iridium oxide in acidic oxygen evolution reactions are enhanced. The Ru0.5Ir0.5O2 catalyst exhibits good activity and stability under acidic conditions, forming more high oxidation state Ru active sites.

NATURE COMMUNICATIONS (2023)

Article Chemistry, Multidisciplinary

The operation active sites of O2 reduction to H2O2 over ZnO

Yunjie Zhou, Liang Xu, Jie Wu, Wenxiang Zhu, Tiwei He, Hao Yang, Hui Huang, Tao Cheng, Yang Liu, Zhenhui Kang

Summary: We demonstrate an ideal ZnO@ZnO2 electrocatalyst for efficient oxygen reduction to hydrogen peroxide in a neutral medium. The in situ growth of ZnO2 on ZnO forms heterogeneous interfaces, weakening the binding energies of OOH* and O*. In a 0.1 M K2SO4 electrolyte, ZnO@ZnO2 exhibits nearly 100.0% selectivity for H2O2 production and a production rate of 5.47 mol g(cat)(-1) h(-1) at 0.1 V vs. RHE, with a Faraday efficiency of approximately 95.5%.

ENERGY & ENVIRONMENTAL SCIENCE (2023)

Article Multidisciplinary Sciences

Coherent hexagonal platinum skin on nickel nanocrystals for enhanced hydrogen evolution activity

Kai Liu, Hao Yang, Yilan Jiang, Zhaojun Liu, Shumeng Zhang, Zhixue Zhang, Zhun Qiao, Yiming Lu, Tao Cheng, Osamu Terasaki, Qing Zhang, Chuanbo Gao

Summary: This study reports a method for synthesizing metastable hexagonal Pt nanostructures on 3d transition metal nanocrystals without involving galvanic replacement reaction, expanding the frontier of phase-replication synthesis. Compared to noble metal substrates, the 3d transition metal substrate has more crystal phases and lower cost, providing the hexagonal Pt skin with compressive strains and programmable charge density, making it particularly suitable for the alkaline hydrogen evolution reaction. The energy barriers are greatly reduced, resulting in high activity for hydrogen evolution. This strategy paves the way for tailored electronic properties of metastable noble metal catalysts for efficient and cost-effective energy conversion.

NATURE COMMUNICATIONS (2023)

Article Chemistry, Physical

DFT-ReaxFF hybrid molecular dynamics investigation of the decomposition effects of localized high-concentration electrolyte in lithium metal batteries: LiFSI/DME/TFEO

Yiming Lu, Qintao Sun, Yue Liu, Peiping Yu, Yanyan Zhang, Jiachen Lu, Haochen Huang, Hao Yang, Tao Cheng

Summary: Due to their potential use in portable applications such as electric vehicles, lithium-metal batteries (LMBs) have attracted attention for their low electrochemical potential and high theoretical specific energy. However, the uncontrolled growth of lithium dendrites during cycling has been a challenge. Recently, the concept of using localized high-concentration electrolytes (LHCEs), achieved by diluting high concentration electrolytes with inert solvents, has shown promise in enabling dendrite-free cycling of LMBs. In this study, the reactions of lithium bis(fluorosulfonyl)imide (LiFSI) in a mixture of dimethoxyethane (DME)/tris(2,2,2-trifluoroethyl) orthoformate (TFEO) electrolyte at a lithium metal anode were investigated. The formation mechanism of the solid electrolyte interface (SEI) was studied using a hybrid ab initio and reactive force field (HAIR) method. The results revealed important initial reduction reactions of LiFSI, TFEO, and DME, leading to the formation of a LiF-rich SEI inorganic inner layer (IIL) and unsaturated carbon products from TFEO. These findings can provide valuable insights for the future design of improved electrolytes.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2022)

No Data Available