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Dual polarization strategy to enhance CH_(4) uptake in covalent organic frameworks for coal-bed methane purification

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Chinese Chemical Letters 2024年第8期35卷 545-548页

作者： Junhua Wang Xin Lian Xichuan Cao Qiao Zhao Baiyan Li xian-he bu School of Materials Science and Physics China University of Mining and TechnologyXuzhou 221116China School of Chemical Engineering and Technology China University of Mining and TechnologyXuzhou 221116China School of Materials Science and Engineering National Institute for Advanced MaterialsTKL of Metal and Molecule-Based Material ChemistryNankai UniversityTianjin 300350China

The purification of low-grade coal-bed methane is extremely important,but challenging,due to the very similar physical properties of CH_(4)and ***,we proposed a dual polarization strategy by employing triazine and polyfluoride sites to construct polar pores in COF materials,achieving the efficient separa-tion of CH_(4)from *** expected,the dual polarized F-CTF-1 and F-CTF-2 exhibit higher CH_(4)adsorption capacity and CH_(4)/N_(2)selectivity than CTF-1 and CTF-2,***,the CH4 uptake capacity and CH_(4)/N_(2)selectivity of F-CTF-2 is 1.76 and 1.42 times than that of *** work not only developed promising COF materials for CH4/N_(2)separation,but also provided important guidance for the separation of other adsorbates with similar properties.

关键词： Dual polarization strategy Covalent organic frameworks(COFs) Coal-bed methane purification Chemical/thermal stability Cycling stability

Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting

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Nano Research 2024年第3期17卷 1114-1122页

作者： Chao-Peng Wang Hao Sun Gang Bian Jia-Xi Wang Xixi Pang Guoqi Wang Jian Zhu xian-he bu School of Materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Tianjin Key Laboratory of Metal and Molecule-Based Material Chemistry Nankai UniversityTianjin 300350China Tianjin Key Laboratory for Rare Earth Materials and Applications Nankai UniversityTianjin 300350China

Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient ***,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)*** particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 ***,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(heR),leading to successful overall water splitting powered by a 1.5 V *** study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.

关键词： layer-by-layer(LbL)assembly layered double hydroxides(LDH) two-dimensional(2D)electrocatalysts oxygen evolution reaction(OER) water splitting

Rational design of ZnCdS/TpPa-1-COF heterostructure photocatalyst by strengthening the interface connection in solar hydrogen production reactions

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Nano Research 2024年第3期17卷 1027-1034页

作者： Di Yang Zhi-Gang Li Xinghao Zhang Zenghuan Ren Weihan Lu Haining Liu Xiaomeng Guo Jijie Zhang xian-he bu Tianjin Key Laboratory of Metal and Molecule-Based Material Chemistry School of Materials Science and EngineeringNankai UniversityTianjin 300350China College of Chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China State Key Laboratory of Elemento-Organic Chemistry College of ChemistryNankai UniversityTianjin 300071China

ZnCdS quantum dots(QDs)are highly coveted in photocatalysis research for their exceptional visible-light responses and high light-absorption ***,their practical application is hindered by their tendency to aggregate,due to having high surface *** address this issue,herein,a heterostructure is synthesized by growing ZnCdS QDs with a size of approximately 5 nm onto the surface of a two-dimensional(2D)covalent organic framework(COF),*** approach suppresses the aggregation of the QDs and improves their *** ZnCdS/TpPa-1-COF composite exhibited a peak hydrogen evolution rate of 6244.16μmol·g^(-1)·h^(-1),which was 2.89 and 4.18 times greater than that of ZnCdS and TpPa-1-COF,*** zero-dimensional/two-dimensional(0D/2D)heterojunction formed by ZnCdS and TpPa-1-COF generates a strong interfacial force,which is attributed to the intimate contact between the *** connections accelerate charge separation,improve the utilisation of reduced electrons,and reduce the extent of agglomeration of the ZnCdS QDs,thereby resulting in high hydrogen production activity of the ***,the photocatalytic mechanism is studied using Kelvin probe force microscopy and theoretical *** study offers a novel approach for creating sulfide photocatalysts and is crucial for investigating the potential practical applications of the related photocatalysts.

关键词： covalent organic frameworks quantum dots photocatalysis hydrogen generation heterojunction

Post-synthetic modifications of MOFs by different bolt ligands for controllable release of cargoes

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Chinese Chemical Letters 2024年第10期35卷 430-433页

作者： Hao Wang Meng-Qi Pan Ya-Fei Wang Chao Chen Jian Xu Yuan-Yuan Gao Chuan-Song Qi Wei Li xian-he bu College of New Materials and Chemical Engineering Beijing Key Lab of Special Elastomeric Composite Materials Beijing Institute of Petrochemical Technology School of Materials Science and Engineering National Institute for Advanced Materials TKL of Metal and Molecule-Based Material Chemistry Nankai University College of Chemical Engineering Inner Mongolia University of Technology

Post-synthetic modifications(PSM) have drawn great attention as a vigoroso tool to tune or enhance the performance of metal-organic frameworks(MOFs). However, the current PSM method usually have to sacrifice the porosity of MOFs to enrich their functionality, such as pore space partition(PSP) and postsynthetic elimination and insertion(PSE&I), causing a trade-off in this aspect. To address this issue, we herein propose a new PSM strategy of using the size-matching ligands as the bolts to lock MOFs' pores,which could be anchored onto open metal sites(OMSs) after guest loading through a stepwise manipulation. As a result, the loaded cargoes undergo a controlled releasing process with respect to different bolt ligands. Our proposed strategy provides a promising way to balance the functionality and porosity of MOFs.

关键词： Bolting ligand Cargo Control release Metal-organic frameworks Post-synthetic modifications

Donor-acceptor modulation of coordination polymers for effective photothermal conversion

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Science China Chemistry 2024年

作者： Bo Zhang Xing-Wang Li Han Fang Chang-Tai Li Si-Jia Yu Mei-Hui Yu Ze Chang xian-he bu School of Materials Science and Engineering Nankai University State Key Laboratory of Elemento-Organic Chemistry Nankai University

The targeted construction of donor-acceptor（D-A） materials featuring efficient photothermal（PT） conversion properties has been an attractive but challenging goal. herein, a new series of coordination polymers（CPs） featuring different PT performances were constructed with flexible linker 1,1′-Ferrocenedicarboxylic acid（FCA） and 2,4,6-tri（pyridin-4-yl）-1,3,5-triazine（TPT） as acceptor and donor molecules including coronene and tetrathiafulvalene（TTF）. Based on the flexible configurations of FCA ligand and the directing of donor dependent D-A interactions, the structures of TF-1 to TF-3 featuring distinctive dimension were obtained based on Cd（II） ions for investigating the PT property in configurational perspectives. A systematic investigation of the PT properties of the CPs was performed. Notably, TF-3 exhibits the finest PT conversion effect under the irradiation of 560 nm laser, while TF-2 shows optimal PT conversion under 808 nm laser irradiation required for biological PT therapy,illustrating the correlation between the structural and component features of the CPs and their PT performances. Furthermore,Zn（II） as bio-friendly ion was utilized to construct hypotoxic TF-4 that reveals similar structure to that of TF-2 for potential application. Polydimethylsiloxane（PDMS） patches doped with TF-4 exhibits considerable NIR PT conversion effect under808 nm, represented by the nearly 80 °C temperature increased in 120 s for TF-4@PDMS patch（1.2 wt%） under 0.9 W cm-2irradiation, the results of which herein indicate the potential of D-A CPs as versatile platform for the modulation of PT materials.

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‘All-in-one’ strategy for metalla[3]catenanes and ring-in-ring complex

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National Science Review 2021年第5期8卷 14-15页

作者： xian-he bu School of Materials Science and Engineering National Institute for Advanced MaterialsNankai University

Research into mechanically interlocked molecules, such as catenanes, rotaxanes and molecular knots, has been gaining momentum in recent decades, not only because of their intriguing structures and topological importance, but also because of their important applications as molecular machines and nanoscale devices [1,2]. In addition to traditional organic macrocycles based on covalent bonds,

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Removable urea solves the COF dilemma

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Science China Chemistry 2022年第7期65卷 1221-1222页

作者： xian-he bu School of Materials Science and Engineering Nankai UniversityTianjin 300350China

Since the first report in 2005 [1], covalent organic frameworks(COFs) have become a major platform for materials design owing to their high crystallinity, low density, large surface area, tailorable pore aperture, and versatile molecular architecture, which has attracted wide attention in gas storage, separation, electronics, and catalysis [2–5].

关键词： versatile catalysis separation

Recent advances and perspectives of metal/covalent-organic frameworks in metal-air batteries

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Journal of Energy Chemistry 2021年第12期30卷 113-129,I0003页

作者： Ming Zhong Ming Liu Na Li xian-he bu School of Materials Science and Engineering Tianjin Key Laboratory of Metal and Molecule-Based Material ChemistryNankai UniversityTianjin 300350China State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals Lanzhou University of TechnologyLanzhou 730050GansuChina College of Chemistry Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Nankai UniversityTianjin 300071China

Metal-air batteries(MABs)have attracted considerable attention as a novel energy technology that can alleviate the severe energy crisis and environmental *** primary processes,including oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)occur on the air cathode and dominate the battery performance during battery charging and ***,metal-organic frameworks(MOFs)and covalent-organic frameworks(COFs)emerge as promising cathode catalysts due to their structure and composition *** unique characteristics of MOFs and COFs contribute to improved *** review mainly summarizes the recent applications of MOFs and COFs in a series of MABs,mainly including lithium-and zinc-air ***,some critical issues are emphasized regarding MOFs and COFs used in other MABs limited progress,their fabrication and alternatives to potential problems.

关键词： Metal-organic frameworks Covalent-organic frameworks Li-air batteries Zn-air batteries Active sites

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构筑未来:框架化学的研究前沿与产业化展望

中国科学：化学 2024年第6期54卷 815-821页

作者：岳衎丁三元雷浩卜显和陈小明付雪峰国家自然科学基金委员会化学科学部北京100085 华南理工大学前沿软物质学院广州510640 兰州大学功能有机分子化学国家重点实验室化学化工学院兰州730000 暨南大学广东省功能配位超分子材料及应用重点实验室化学与材料学院广州510632 南开大学材料科学与工程学院天津300350 中山大学化学学院广州510275

基于“框架化学的基础及应用研究”研讨会,本文阐述了“框架化学”的科学内涵,从框架结构的设计合成、精确表征、高性能化和产业应用四个方面综述了框架化学领域的主要研究进展,凝练了该领域的关键科学问题,并提出了面向国家需求和产业... 详细信息

基于“框架化学的基础及应用研究”研讨会,本文阐述了“框架化学”的科学内涵,从框架结构的设计合成、精确表征、高性能化和产业应用四个方面综述了框架化学领域的主要研究进展,凝练了该领域的关键科学问题,并提出了面向国家需求和产业发展的重点发展方向.

关键词：框架化学多孔材料金属-有机框架共价有机框架超分子有机框架