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Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO2 reduction

Science China Chemistry 2025年

作者： Xinxin Wang Yucheng Jin Xiya Yang Qingyu Luan Tianyu Wang Dongdong Qi Kang Wang jianzhuang jiang College of Chemistry and Materials Science Anhui Normal University Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry and Chemical Engineering School of Chemistry and Biological EngineeringUniversity of Science and Technology Beijing

Lead halide perovskite quantum dots（LHP QDs） have been revealed to possess great potential in photocatalytic applications including CO2reduction, which however suffer from poor stability. Herein, a high crystalline hydrazine-linked three-dimensional（3D） covalent organic framework, USTB-17, was fabricated from the reaction between 12-connected building block and 4-connected 3,5,7-tetrakis（4-aldophenyl）-adamantane. Post-modification with Ni2+affords the metallic framework USTB-17（Ni）followed by sequential deposition of the CH3NH2PbI3（MAPbI3） perovskite QDs into its pores, generating the USTB-17（Ni）@MAPbI3composite. Powder X-ray diffraction analysis together with theoretical simulations and transmission electron microscopy discloses the crystalline nature of USTB-17, USTB-17（Ni）, and USTB-17（Ni）@MAPbI3with an unprecedented noninterpenetrated hpt topology. The close contact of QDs inside the COF pores with the Ni catalytic site locating at the pore surface of COF allows a rapid transfer of the photogenerated electrons in QDs to the Ni catalytic sites, enhancing the photocatalytic activity for CO2reduction. This endows USTB-17（Ni）@MAPbI3with efficient photocatalysis performance for photocatalytic CO2reduction with CO generation rate of 365 μmol g-1h-1and CO selectivity up to 96% under visible-light irradiation, 7 times higher than that of USTB-17（Ni）. After four cycles of reactions, the photocatalytic CO generation rate remains almost unchanged, demonstrating its excellent cycle stability.

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Atomic CoN_(3)S_(1) sites for boosting oxygen reduction reaction via an atomic exchange strategy

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Nano Research 2022年第3期15卷 1803-1808页

作者： Qianjun Zhi Rong jiang Wenping Liu Tingting Sun Kang Wang jianzhuang jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

It is vitally important to develop high-efficiency low-cost catalysts to boost oxygen reduction reaction(ORR)for renewable energy ***,an A-CoN_(3)S_(1)@C electrocatalyst with atomic CoN_(3)S_(1)active sites loaded on N,S-codoped porous carbon was produced by an atomic exchange *** constructed A-CoN_(3)S_(1)@C electrocatalyst exhibits an unexpected half-wave potential(0.901 V *** hydrogen electrode)with excellent durability for ORR under alkaline conditions(0.1 M KOH),superior to the commercial platinum carbon(20 wt.%Pt/C).The outstanding performance of A-CoN_(3)S_(1)@C in ORR is due to the positive effect of S atoms doping on optimizing the electron structure of the atomic CoN_(3)S_(1)active ***,the rechargeable zinc-air battery in which both A-CoN_(3)S_(1)@C and IrO_(2)were simultaneously served as cathode catalysts(A-CoN_(3)S_(1)@C&IrO_(2))exhibits higher energy efficiency,larger power density,as well as better stability,compared to the commercial Pt/C&IrO_(2)-based zinc-air *** present result should be helpful for developing lower cost and higher performance ORR catalysts which is expected to be used in practical applications in energy devices.

关键词： atomic sites oxygen reduction reaction CoN_(3)S_(1) zinc-air battery

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In-situ growth of ZnS/FeS heterojunctions on biomass-derived porous carbon for efficient oxygen reduction reaction

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Journal of Energy Chemistry 2020年第8期29卷 79-85,I0003页

作者： Rong jiang Xin Chen Jinxia Deng Tianyu Wang Kang Wang Yanli Chen jianzhuang jiang Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijing 100083China School of Materials Science and Engineering China University of Petroleum(East China)Qingdao 266580ShandongChina

It is an urgent task to develop highly efficient non-noble metal electrocatalysts in the direction of ORR,but still a huge and long-term ***,an efficient one-step pyrolysis of Sichuan pepper powder,2,2-bipyridine,FeCl3,Na SCN,and ZnCl2 at 900℃ provides the FeS/ZnS@N,S-C-900 hybrid *** electron microscopy(TEM)images and Mott-Schottky curves clearly reveal the in-situ constructed abundant FeS/ZnS-based p-n junctions dispersed on the biomass-derived porous carbon surface of FeS/ZnS@N,*** as-prepared FeS/ZnS@N,S-C-900 hybrid exhibits superior ORR performance in comparison with Pt/C in 0.1 M KOH with high onset(Eonset)and half-wave potentials(E1/2)of 1.00 and 0.880 V ***,large limiting current density(JL)of 5.60 mA cm-2,and robust durability and methanol ***,upon the light irradiation,FeS/ZnS@N,S-C-900 produces a photocurrent as high as ca.0.3μA cm-2,resulting in further improvement over Eonset,E1/2,and JLof FeS/ZnS@N,S-C-900 to1.10 V ***,0.885 V ***,and 6.02 mA *** in combination with theoretical calculations demonstrate the significant effect of FeS/ZnS heterojunction on the enhanced ORR catalytic activity of FeS/ZnS@N,*** work is useful for the development of advanced heterojunction-based ORR catalysts for various energy conversion devices.

关键词： Heterojunction Oxygen reduction reaction Photo-responsive electrocatalyst Biomass-derived carbon

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Topochemical polymerization of hydrogen-bonded organic framework for supporting ultrafine palladium nanoparticles

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Science China Chemistry 2023年第7期66卷 2019-2027页

作者： Xu Ding Bin Han Baoqiu Yu Hailong Wang jianzhuang jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Topochemical polymerization of molecular crystals into porous materials is of significance due to their promising applications in the field of adsorption and catalysis,yet rarely reported due to the synthesis ***,a hydrogen-bonded organic framework(HOF-45)has been fabricated by the crystallization of a cage-like building block containing three alkynyl *** exhibits almost mesoporous structure demonstrated by single crystal X-ray diffraction ***-driven topochemical polymerization of HOF-45 with ethanedithiol covalently links alkynyl groups in HOF-45,generating a hydrogen-bond and covalentbond cross-linked material(HOF-45C).In contrast to HOF-45,cross-linked HOF-45C retains the crystalline nature and displays improved solution resistence according to the powder X-ray diffraction *** particular,HOF-45C is able to support the growth of ultrafine palladium nanoparticles with the average size of ca.1.9 nm for rapidly promoting the degradation of nitrophenol,methyl orange,and congo red with the help of NaBH_(4)as well as Suzuki-Miyaura coupling *** work inputs a new idea on the HOFs application in preparing covalent-linked porous organic materials.

关键词： hydrogen-bonded organic frameworks topochemical polymerization palladium nanoparticles nitrophenol degradation organic dyes degradation Suzuki-Miyaura coupling reaction

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Synthetic porphyrin chemistry in China

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Science China Chemistry 2018年第5期61卷 511-514页

作者： Chengjie Li Junlong Zhang Jianxin Song Yongshu Xie jianzhuang jiang Key Laboratory for Advanced Materials and Institute of Fine Chemicals Shanghai Key Laboratory of Functional Materials Chemistry School of Chemistry & Molecular Engineering East China University of Science & Technology Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular Engineering Peking University Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research (Ministry of Education of China) Key Laboratory of Application and Assemble of Organic Functional Molecules Hunan Normal University Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry University of Science and Technology Beijing

Porphyrins are a class of heterocyclic macrocycles,containing four pyrrolic subunits interconnected at theα-positions with four methine（=CH-）groups.

关键词： In Figure Synthetic porphyrin chemistry in China NIR OC DDQ

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Density functional theory study on organic semiconductor for field effect transistors: Symmetrical and unsymmetrical porphyrazine derivatives with annulated 1,2,5-thiadiazole and 1,4-diamyloxybenzene moieties

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Science China Chemistry 2009年第6期52卷 840-848页

作者： CAI Xue ZHANG YueXing QI DongDong jiang jianzhuang Department of Chemistry University of Science and Technology BeijingBeijing 100083China Department of Chemistry Mudanjiang Normal CollegeMudanjiang 157012China Department of Chemistry Shandong UniversityJinan 250100China

Density functional theory (DFT) calculations were carried out to investigate the organic field effect transistor (OFET) performance of the symmetrical metal-free tetrakis (1,2,5-thiadiazole) porphyrazine (S4)PzH2 and tetrakis (1,4-diamyloxybenzene) (A4)PzH2 as well as the low-symmetry metal-free porphy- razine with annulated 1,2,5-thiadiazole and 1,4-diamyloxybenzene groups in the ratio 2:2 (cis) and 1:3, that is, (cis-S2A2)PzH2 and (SA3)PzH2, (S = 1,2,5-thiadiazole ring, A = annulated 1,4-diamyloxy-benzene ring, Pz = porphyrazine) in terms of the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy, ionization energy (IE), electron affinity (EA), and their reorganization energy (λ) during the charge-transport process. On the basis of Marcus electron transfer theory, electronic couplings (V) and field effect transistor (FET) properties for the four compounds with known crystal structure have been calculated. The electron transfer mobility (μ -) is revealed to be 0.056 cm2·V-1·s-1 for (S4)PzH2. The hole transfer mobility (μ+) is 0.075, 0.098, and 8.20 cm2·V-1·s-1 for (cis-S2A2)PzH2, (SA3)PzH2, and (A4)PzH2, respectively. The present work represents the theoretical effort towards understanding the OFET properties of symmetrical and unsymmetrical porphyrazine derivatives with annulated 1,2,5-thiadiazole and 1,4-diamyloxybenzene.

关键词： porphyrazine organic field effect transistor reorganization energy density functional theory

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Chiral porphyrin assemblies

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Aggregate 2023年第1期4卷 27-40页

作者： Li Zhang TianyuWang jianzhuang jiang Minghua Liu Beijing National Laboratory for Molecular Science(BNLMS) CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijingP.R.China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijingP.R.China

Porphyrins are among the most important macrocycles because they perform many essential functions in living systems and serve as building blocks in many functional *** the chirality into porphyrins can aid biomimetic research and the exploration of new functional *** this review,recent developments in chiral porphyrin assemblies are *** review is mainly divided into two sections:the different strategies for constructing chiral porphyrin assemblies and the *** formation of chiral porphyrin assemblies can be from porphyrin molecules substituted with chiral groups;achiral porphyrins induced by chiral additives and spontaneous deracemizations of achiral porphyrins during the *** also provide an overview of the applications of chiral porphyrin assemblies in chiral sensing,asymmetry catalysis,circularly polarized luminescence,and so *** further challenge in the field is discussed.

关键词： chiral circularly polarized luminescence helical porphyrins self-assembly

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Advances in gas sensors of tetrapyrrolato-rare earth sandwich-type complexes——Commemorating the 100th anniversary of the birth of Academician Guangxian Xu

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Journal of Rare Earths 2021年第2期39卷 113-120页

作者： Xiangjie Tang Qi Liu Chuangyu Wei Xuehui Lv Zhicheng Jin Yanli Chen jianzhuang jiang School of Materials Science and Engineering College of ScienceChina University of Petroleum(East China)Qingdao 266580China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijing 100083China

In recent years,sandwich-type rare earth tetrapyrrole derivatives,have attracted more and more attention as material for conductimetric *** have not only great chemical stability and processability,but also flexible molecular structure,which is a key to adjustable semiconductor *** this mini review,we focus mainly on the development of tetrapyrrolato-rare earth sandwich-type complexes as the semiconducting active layer in the gas sensors published in the last ten years(2010-2020).The main part includes two *** the single component gas sensing of sandwich rare earth tetrapyrrole complexes,we describe the influence factors of the single-component semiconducting active layer on the sensing performance of tetrapyrrolato-rare earth sandwich-type complexes,including substituents,central metals and π-conjugate *** the multi-component gas sensors,the synergistic effect between tetrapyrrolato-rare earth sandwich-type complex and other materials on improving sensitivity and conductivity has been discussed briefly.

关键词： Sandwich-type rare earth tetrapyrrole complex Phthalocyanine Gas sensor Rare earths

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High Fluorescence Porous Organic Cage for Sensing Divalent Palladium Ion and Encapsulating Fine Palladium Nanoparticles

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Chinese Journal of Chemistry 2022年第3期40卷 385-391页

作者： Huimin Ren Chao Liu Xu Ding Xianzhang Fu Hailong Wang jianzhuang jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Porous organic cages(POCs)as an innovative type of porous molecular materials enable multifunctional ***,a fluorescence POC(denoted as 1)has been constructed by means of 5/5'-((2/5-dimethoxy-l/4-phenylene)bis(ethyne-2/1-diyl))diiso-phthalaldehyde condensing with cyclohexanediamine enantiomer with the aid of trifluoroacetic acid.1 exhibits the permanent void and prominent fluorescence with relative quantum yield of 73%confirmed by gas sorption and emission experiments,***,this organic cage is capable of sensing diavalent Pd2+according to the fluorescence response to the addition of various metal *** dispersion of 1 in methanol containing palladium acetate was stirred at 25℃and then 80℃to reduce Pd2+ions into nanoparticles(NPs),leading to the composite(Pd@l)composed of fine Pd NPs with the size of co.1.8 *** catalytic nature of Pd@l over NaBH4 promoted the degeneration of nitrobenzene and congo *** work introduces one new case of POCs with versatile properties and functions,including ion fluorescence recognition,fine Pd NPs stabilizer,and gas adsorption,enriching the family of POC-based materials.

关键词： Catalysis Fluorescence recognition Nanoparticles Cage compounds Palladium

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High Sensitive Ambipolar Response towards Oxidizing NO2 and Reducing NH3 Based on Bis（phthalocyaninato） Europium Semiconductors

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Chinese Journal of Chemistry 2016年第10期34卷 975-982页

作者： Xia Kong Zhen Dong Yanling Wu Xiyou Li Yanli Chen jianzhuang jiang School of Science China University of Petroleum (East China) Qingdao Shandong 266580 China Beymg Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry University of Science and Technology Beijing Beijing 100083 China

High sensitive chemical sensors towards NO2 and NH3 based on the self-assembled nanostructures of the heteroleptic and homoleptic bis（phthalocyaninato） europium complexes with octanaphthoxy phthalocyaninato ligands named Eu（Pc）[Pc（ONh）8] （1） and Eu[Pc（ONh）8]2 （2） [Pc = unsubstituted phthalocyaninate; Pc（ONh）8 = 2,3,9,10,16,17,23,24-octanaphthoxy phthalocyaninate] have been developed. The good conductivity, high crystal- linity and large specific surface area for the self-assemblies of 1 render it excellent sensing property for either electron-accepting gas NO2 in 50--250 ppb range or electron-donating gas NH3 in 2.5--12.5 ppm range due to the optimized molecular packing in the uniform-sized nanopartieles depending on the effective intermolecular interaction between double-decker molecules, among the best results of phthalocyanine-based chemical sensors for detection of NO2 and NH3 at room temperature. Interestingly, self-assemblies of I exhibited n-type response to NO2 and p-type response to NH3, which is the first example of ambipolar charge-transporting gas sensors fabricated from single- component organic semiconductors. However, the self-assemblies of 2 with sixteen bulky naphtboxy groups at the periphery of two Pc rings only present an n-type response to strong oxidant gas NO2 in a relatively high concentration of 0.5 - 1.5 ppm, while are insensitive to weak reducing gas NH3 due to the existence of great steric hindrance from bulky naphthoxy groups and more traps and/or defects in self-assemblies.

关键词： phthalocyanine double-decker gas sensor self-assemblies ambipolar semiconductor

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