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Multi-stimuli-responsive aggregation-induced emission copper iodide cluster

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Science China chemistry 2024年第4期67卷 1193-1197页

作者： Bo Li Yuan-Yuan Liu Peng Luo Ye-Ru Liu Ying-Jun Chen Kai Li Shuang-Quan Zang College of chemistry and Pharmacy Engineering Nanyang Normal UniversityNanyang 473061China green catalysis Center and College of chemistry Zhengzhou UniversityZhengzhou 450001China

Stimuli-responsive luminescent materials have attracted significant attention in the development of smart photoactive materials for both fundamental research and technological *** this work,a new copper iodide cluster(1)with aggregationinduced emission(AIE)characteristic,was obtained combining Cu_(4)I_(4) core with rhodamine B derivative ligand.1 has reversible and distinct multi-stimuli-responsive luminescence for external temperature,volatile organic compound,and mechanical ***,1 exhibited unusual large blue shift(84 nm)after being ground,which originated from the change of intermolecular ***,1 exhibits high oxygen quenching efficiency for 82.2% at 1 *** studies showed that the multi-stimuli-responsive luminescence properties of 1 can be attributed to the regulation of cluster-centered luminescence process,metal-to-ligand charge transfer process,halide-to-metal charge transfer luminescence process and aggregationinduced barrier to oxygen *** work not only reports an AIE copper iodide cluster,but also provides a new strategy to develop multi-stimuli-responsive luminescence materials.

关键词： copper iodide cluster aggregation-induced emission multi-stimuli-response

Electronic structure regulation and built-in electric field synergistically strengthen photocatalytic nitrogen fixation performance on Ti-BiOBr/TiO_(2)heterostructure

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Rare Metals 2024年第3期43卷 1125-1138页

作者： Ru-Qi Li Yu-Jie Bian Chun-Ming Yang Li Guo Tao-Xia Ma Chuan-Tao Wang Feng Fu Dan-Jun Wang College of chemistry and Chemical Engineering Yan’an UniversityYan’an Key Laboratory of Green Catalysis and Quality Improvement and Utilization of Low Rank CoalYan’an716000China

At present,industrial synthetic ammonia was still obtained through the Hubble-Bosch process,with large energy *** is a research hotspot to realize green synthetic ammonia by using solar *** difficulty of photocatalytic ammonia synthesis was that the photo-excited electrons have not enough energy to active N≡*** this study,Ti was doped into BiOBr by one-step hydrothermal method,which was oxidized into TiO_(2)when the doping amount reaches the maximum,in situ forming Ti_(0.31)B_(0.69)OB/TiO_(2)*** from the synergistic effect of Ti doping and S-scheme heterojunction,the synthetic ammonia efficiency of Ti_(0.31)B_(0.69)OB/TiO_(2)-11.96 reached 1.643 mmol·g_(cat)^(-1)at mild conditions and without hole scavenger for up to 7 h,the efficiency of synthetic ammonia is 115 times,10.5 times and 3.3 times of that of BiOBr,Ti_(0.31)B_(0.69)OB and TiO_(2),***,DFT calculation confirms that Ti doping accurately refine the electronic structure of BiOBr,facilitate nitrogen adsorption activation and reduce hydrogenation reaction energy barrier,thus accelerating the reaction kinetics of photocatalytic nitrogen reduction(NRR),Meanwhile,constructing S-scheme heterojunction boosts the separation and transfer of photogenerated electron-hole pairs,improving the reduction ability of electrons in the conduction band of TiO_(2)and the oxidation ability of holes in the valence band of Ti_(0.31)B_(0.69)OB.

关键词： S-scheme heterostructure Electronic structure regulation Built-in electric field Synergistical stren4gthening Photocatalytic nitrogen fixation

Enabling low-cost decentralized power reserves adopting carbon dioxide for green methane exchange in stabilized clathrate adsorbent

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Journal of Energy chemistry 2024年第10期97卷 438-443页

作者： Lucas Hanssens Maarten Houlleberghs C.Vinod Chandran Geert Watson Sambhu Radhakrishnan Pascal Van Der Voort Joeri F.M.Denayer Christine E.A.Kirschhock Johan A.Martens Eric Breynaert centre for Surface chemistry and catalysis-Characterization and Application Team (COK-KAT) NMR/X-Ray Platform for Convergence Research (NMRCoRe) centre for Ordered Materials Organometallics and Catalysis (COMOC) Department of Chemistry Ghent University Department of Chemical Engineering Vrije Universiteit Brussel

*** circular methane energy systems In recent decades,methane-based energy systems have rapidly gained traction across the globe because of the increasing availability of low-cost methane production ***,fossil methane... 详细信息

关键词： Long duration energy storage green methane Carbon neutrality Confined clathrate hydrates CH4 /CO2 exchange Direct gas exchange ENERGY-STORAGE CONFINED NANOSPACE TO-METHANE GAS MECHANISMS ADSORPTION HYDROGEN

Constructing energetic covalent organic frameworks with high stability and low sensitivity

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Chinese Chemical Letters 2024年第3期35卷 544-548页

作者： Hui-Min Guo Xiao-Yu Dong Shan Wang Qian-You Wang Shuang-Quan Zang Henan Key Laboratory of Crystalline Molecular Functional Materials Green Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China

Developing new functional explosives that display high stability,good energy performance,and low sensitivity are one of the key directions of energetic materials *** this work,two-dimensional(2D)Schiff-based energetic covalent organic frameworks(COFs)are prepared based on triaminoguanidine salts with different anions as building *** from the robust covalent bond in 2D extended polygons and strongπ-πinteractions in the eclipsed interlayers,the synthesized energetic COFs showed higher thermal stability and lower mechanical sensitivity than their precursor *** importantly,incorporating triaminoguanidine salts into COFs effectively increase the corrosion resistance to metal under high humidity conditions,which is due to the imine moieties in COFs functioning asπacceptors and offering strong bonding with metallic *** work provides a new pathway for the development of high-performance energetic materials.

关键词： Covalent organic frameworks Energetic materials High thermal stability Low sensitivity Corrosion resistance

Grapevine-like high entropy oxide composites boost high-performance lithium sulfur batteries as bifunctional interlayers

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green Energy & Environment 2024年第3期9卷 565-572页

作者： Huarong Fan Yubing Si Yiming Zhang Fulong Zhu Xin Wang Yongzhu Fu College of chemistry and Center of green catalysis Zhengzhou UniversityZhengzhou450001China School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu611731China

Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand ***,their commercial applicability is hampered by hysteretic electrode reaction kinetics and the shuttle effect of lithium polysulfides(LiPSs).In this work,an interlayer consisting of high-entropy metal oxide(Cu_(0.7)Fe_(0.6)Mn_(0.4)Ni_(0.6)Sn_(0.5))O_(4) grown on carbon nanofibers(HEO/CNFs)is designed for *** CNFs with highly porous networks provide transport pathways for Li^(+) and e^(-),as well as a physical sieve effect to limit LiPSs *** particular,the grapevine-like HEO nanoparticles generate metal-sulfur bonds with LiPSs,efficiently anchoring active *** unique structure and function of the interlayer enable the LSBs with superior electrochemical performance,i.e.,the high specific capacity of 1381 mAh g^(-1) at 0.1 C and 561 mAh g^(-1) at 6 *** work presents a facile strategy for exploiting high-performance LSBs.

关键词： Electrospun carbon nanofibers Grapevine-like morphology Hierarchical physical sieve effect High-entropy induced chemisorption Lithium-sulfur battery

One-shot synthesis of heavy-atom-modified carbazole-fused multi-resonance thermally activated delayed fluorescence materials

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Science China Materials 2024年第9期67卷 2789-2795页

作者： Jia-Jun Hu Jia-Qi Liang Zhi-Ping Yan Hua-Xiu Ni Xiang-Ji Liao You-Xuan Zheng State Key Laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China green catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou450001China

Efficient multi-resonance thermally activated delayed fluorescence(MR-TADF)materials hold significant potential for applications in organic light-emitting diodes(OLEDs)and ultra-high-definition ***,the stringent synthesis conditions and low yields typically associated with these materials pose substantial challenges for their practical *** this study,we introduce an innovative strategy that involves peripheral modification with sulfur and selenium atoms for two materials,CFDBNS and *** approach enables a directed one-shot borylation process,achieving synthesis yields of 66%and 25%,respectively,while also enhancing reverse intersystem crossing *** emitters exhibit ultra-narrowband sky-blue emissions centered around 474 nm,with full width at half maximum(FWHM)values as narrow as 19 nm in dilute toluene solutions,along with high photoluminescence quantum yields of 98%and 99%in doped films,*** OLEDs based on CFDBNS and CFDBNSe display sky-blue emissions with peaks at 476 and 477 nm and exceptionally slender FWHM values of 23 ***,the devices demonstrate remarkable performances,achieving maximum external quantum efficiencies of 24.1%and 27.2%.This work presents a novel and straightforward approach for the incorporation of heavy atoms,facilitating the rapid construction of efficient MR-TADF materials for OLEDs.

关键词： one-shot synthesis multi-resonance thermally activated delayed fluorescence carbazole-fused dual-boron embedded framework ultra-narrowband emission organic light-emitting diode

Selective synthesis of the B_(11)H_(14)^(-) and B_(12)H_(12)^(2-) borane derivatives and the general mechanisms of the B-H bond condensation

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Science China chemistry 2024年第3期67卷 876-881页

作者： Yi Jing Xinghua Wang Hui Han Xin-Ran Liu Xing-Chao Yu Xi-Meng Chen Donghui Wei Lai-Sheng Wang Xuenian Chen College of chemistry Green Catalysis CenterZhengzhou UniversityZhengzhou 450001China School of chemistry and Chemical Engineering Henan Key Laboratory of Boron Chemistry and Advanced Energy MaterialsHenan Normal UniversityXinxiang 453007China Department of chemistry Brown UniversityProvidenceRI 02912USA

Polyhedral boranes are a class of well-known boron molecular clusters with unique physical and chemical properties,and great efforts have been made in the past decades to find more effective synthetic ***,the established synthetic methods suffer from low efficiency and low selectivity because the mechanism of the B-H bond condensation reaction,critical for the synthesis of the polyhedral boranes,is not well *** we report highly selective and efficient synthetic methods of the salts of the tetradecahydridoundecaborate(1-)(B_(11)H^(-)_(14)) and dodecahydrido-dodecaborates(2-)(B_(12)H_(12)^(2-)) anions by employing commercially available and inexpensive starting *** theoretical and experimental investigations are carried out to elucidate the reaction *** have found that the nature of the B-H bond condensation is the dihydrogen bonding interaction in which the positively charged hydrogens(bridged hydrogens) play a crucial *** current study has not only led to more effective and selective synthetic methods for B_(11)H^(-)_(14) and B_(12)H_(12)^(2-) but also unveiled the nature of the B-H bond condensation and the general formation mechanisms of polyhedral *** finding will facilitate the development of more effective synthetic methods for polyhedral boranes and spur their wide application.

关键词： Boranes polyhedral boranes dihydrogen bond nucleophilicity

Bimetallic CoNi single atoms supported on three-dimensionally ordered mesoporous chromia: highly active catalysts for n-hexane combustion

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green Energy & Environment 2024年第7期9卷 1122-1137页

作者： Xiuqing Hao Yuxi Liu Jiguang Deng Lin Jing Jia Wang Wenbo Pei Hongxing Dai Beijing Key Laboratory for green catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution Control Key Laboratory of Advanced Functional Materials Education Ministry of China Laboratory of Catalysis Chemistry and Nanoscience Department of Chemical Engineering Faculty of Environment and Life Beijing University of Technology

Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds （VOCs）.In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom （Co1Ni1/meso-Cr2O3） and bimetallic Co and Ni nanoparticle (CoNPNiNP/mesoCr2O3) catalysts adopting the one-pot polyvinyl pyrrolidone （PVP）-and polyvinyl alcohol （PVA）-protecting approaches,*** results indicate that the Co1Ni1/meso-Cr2O3catalyst exhibited the best catalytic activity for n-hexane (C6H14) combustion (T50%and T90%were 239 and 263℃ at a space velocity of 40,000 mL g-1h-1;apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol-1and 4.3×10-7mol g-1cats-1,respectively),which was associated with its higher (Cr5++Cr6+) amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni1was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co1preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen（MvK） mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→COx→CO2and H2O.

关键词： Three-dimensional ordered mesoporous chromium oxide Supported bimetallic single-atom catalyst Cobalt−nickel single atoms n -Hexane combustion Catalytic reaction mechanism

Efficient upcycling of high-density polyethylene into separable cyclic hydrocarbons

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Science China chemistry 2024年第4期67卷 1049-1050页

作者： Shenglu Lu Yanqin Wang State key laboratory of green chemical engineering and industrial catalysis Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

This highlight is inspired by a recent article in Nature Nanotechnology in which Zeng and co-workers[1]from the University of Science and Technology of China reported a strategy for upcycling high-density polyethylene(HDPE)into separable cyclic hydrocarbons under solvent-and hydrogen-free *** work made a significant progress in plastic recycling.

关键词： hydrocarbons cycling high