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Donor-acceptor covalent organic frameworks-confined ultrafine bimetallic Pt-based nanoclusters for enhanced photocatalytic H_(2)generation

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Nano Research 2024年第7期17卷 5835-5844页

作者： Yu Liu Yawen Shi Hua Wang Shengbo Zhang Collaborative Innovation Center of chemical Science and Engineering(Tianjin) Key Laboratory for Green Chemical Technology of the Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China school of Environmental Science and Engineering Tianjin Key Laboratory of Biomass/Wastes UtilizationTianjin UniversityTianjin 300350China

Photocatalytic hydrogen generation from hydrogen storage media is an effective and promising approach for the green hydrogen industry as well as for achieving carbon neutrality ***,the lower photocatalytic efficiency due to the limited light trapping capacity,low electron transfer rate,and severe aggregation of nanoparticles caused by high surface energy seriously restricts their practical ***,we constructed a series of donor–acceptor(D–A)type covalent organic frameworks to confine ultrafine bimetallic Pt-based nanoclusters for photocatalytic hydrogen generation from ammonia borane(AB)*** visible light irradiation at 20℃,PtCo_(2)@covalent organic framework(COF)showed the highest photocatalytic activity with a turnover frequency(TOF)of 486 min−*** and density functional theory(DFT)calculations reveal that the high catalytic activity is mainly attributed to the strong electronic interactions between D–A type COF and ultrafine PtCo_(2)***,the D–A type COF can significantly enhance the light-trapping ability by fine-tuning the electron-acceptor type in the framework,and accelerate the photogenerated electron transfer from D–A type COF to PtCo_(2)nanocluster,which promotes the adsorption and activation of H_(2)O and AB molecules and accelerates hydrogen ***,PtCo_(2)@COF also exhibited ultra-high durability due to the significantly enhanced resistance to nanocluster aggregation caused by the nanopore confinement effect of D–A type *** believe that this work will provide a theoretical guide for the rational design of efficient D–A COFbased catalysts for photocatalysis.

关键词： light trapping electron transfer donor-acceptor covalent organic frameworks(D-A COFs) bimetallic nanoclusters photocatalysis

Prospective life cycle assessment of CO2 conversion by photocatalytic reaction

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Coupling N-doping and confined Co_(3)O_(4) on carbon nanotubes by polydopamine coating strategy for pleiotropic water purification

Green chemical Engineering 2024年第3期5卷 383-389页

作者： Jun-Qi Wang Xiang-Jun Liu Jing-Jing Ma Shuai Zhang Hao-Ran Liu Yong-Li Dong Qing-Yuan Yang school of Human Settlements and Civil Engineering Xi'an Jiaotong University school of chemical Engineering and Technology Xi'an Jiaotong University

CO2conversion is gradually seen as a better way for society to effectively use carbon sources and avoid climate crisis associated with fossil CO2emissions. And the decision to deploy CO2technology scale should be relied on its environmental impact. In this work, life cycle assessment model evaluates the environmental performance of CO2conversion by photocatalytic reaction process with two different catalysts（NiAl-LDH and Co-ZIF-9）. Six impact categories considered in this analysis, including climate change, acidification potential, depletion of abiotic resources, eutrophication potential, ozone layer depletion potential, and photochemical oxidation potential. Results indicated that CO2conversion with Co-ZIF-9 photocatalyst has a better environmental impact than the NiAl-LDH photocatalyst route. Moreover, the Co-ZIF-9 catalyst scenario also has a lower total environmental burden than the conventional CO production route. Sensitivity analysis shows that recycle performance of the catalyst is highly sensitive to the production process in two scenarios. This study could provide a framework for robust decisions in CO2conversion by photocatalytic reaction, which is useful for policymakers to decide the feasibility of industrialization.

关键词： Life cycle assessment (LCA) CO 2 Photocatalytic reaction Sensitivity analysis Uncertainty analysis

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Rare Metals 2024年第7期43卷 3146-3160页

作者： Wen-Long Tu Gang Wang Yue Zhang Hong-Yang Zhu Rong-Rong Du Hong-Yao Zhao Sheng Tang Zeng-Jing Guo Jun Yang Fu Yang Cheng-Zhang Zhu school of Environmental and chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China school of Chemistry and chemical Engineering Liaocheng UniversityLiaocheng 252000China school of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China school of Environmental Science and Engineering Nanjing Tech UniversityNanjing 211816China

The development of effective and sustainable solutions for pleiotropic water purification becomes urgent and *** Fenton-like catalysts for activation of peroxymonosulfate(PMS)to purify organic wastewater show great *** this work,by tuning metal loading with an in-situ polydopamine coating strategy,oxygen vacancy-enriched Co_(3)O_(4) loading on N-doped carbon nanotubes(CNTs)were constructed to enhance PMS activation efficiency for pollutants ***,the obtained modified CNTs afford a well-developed N-containing network structure,which is further endowed with abundant Co(Ⅱ)/Co(Ⅲ)redox cycles and significant metal-carbon *** particular,the surface N doping in CNTs might induce the oriented enrichment of pollutants around the catalyst,which reduces the migration distance and correspondingly improves the utilization of reactive oxidative *** electron transfer efficiency of the catalyst can be further improved by incorporating oxygen vacancy-enriched Co_(3)O_(4).The performance results show that the optimal NC/Co-1 could mineralize 20×10^(-6)of bisphenol A(BPA)by almost 98%in 8 min.A low reaction activation energy(26.05 kJ·mol^(-1))in BPA degradation was demonstrated by the NC/*** importantly,NC/Co-1 can inherit excellent degradation performance towards oxytetracycline,2,4-dichlorophenol,and tetracycline,showing wide practical *** addition,by virtue of the photothermal conversion property,NC/Co-1 achieves an additive function for interfacial solar water evaporation(1.84 kg·m^(-2)·h^(-1),112.51%),showing impressive potential for clean water recovery under complicated environmental pollution conditions.

关键词： Carbon nanotube Advanced oxidation process Co_(3)O_(4) Photothermal conversion Solar water evaporation

Solubility determination and comparison ofβ-HMX and RDX in two binary mixed solvents(acetonitrile+water,nitric acid+water)

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Chinese Journal of chemical Engineering 2024年第5期69卷 238-249页

作者： Yuehua Yao Fan Wang Yinguang Xu Zishuai Xu Lizhen Chen Jianlong Wang school of Chemistry and chemical Engineering North University of ChinaTaiyuan 030051China Gansu Yinguang chemical Industry Group Co.Ltd. Baiyin 730900China

In order to remove hexahydro-1,3,5-trinitro-1,3,5-triazine(RDX),the main impurity,in process of polymorphic transformation of octrahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine(HMX),the solubility ofβ-HMX and RDX in acetonitrile(ACN)+water in the temperature range of 288.15-333.15 K and in nitric acid(HNO_(3))+water in the temperature range of 298.15-333.15 K were measured by laser dynamic *** results showed that the solubility of bothβ-HMX and RDX in binary mixed solvents increased monotonously as the temperature increase at a given solvent composition or with increasing of mole fraction of solvent(ACN and nitric acid).Solubility data were well correlated by the modified Apelblat equation,Jouyban-Acree model,Yaws equation and van't Hoff equation,and the Yaws equation achieved the best fitting results according to the relative error and the mean square error ***,the solubility ofβ-HMX and RDX in binary mixed solvent was compared,based on the solubility difference and the solvent's own properties,the best separation degree ofβ-HMX and RDX was found when the mole fraction of nitric acid was 0.22 at room temperature,which provided data support for HMX crystallization in mixed *** solubility differences between RDX andβ-HMX in mixed solvents were explained from the formation of intermolecular and intramolecular hydrogen bonds.

关键词： Solubility Octrahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine Hexahydro-1,3,5-trinitro-1,3,5-triazine Separation Model Hydrogen bond

Local coordination and electronic interactions of Pd/MXene via dual‐atom codoping with superior durability for efficient electrocatalytic ethanol oxidation

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Carbon Energy 2024年第8期6卷 166-177页

作者： Zhangxin Chen Fan Jing Minghui Luo Xiaohui Wu Haichang Fu Shengwei Xiao Binbin Yu Dan Chen Xianqiang Xiong Yanxian Jin school of Pharmaceutical and chemical Engineering Taizhou UniversityTaizhouZhejiangChina school of Sciences Zhejiang Sci‐Tech UniversityHangzhouZhejiangChina

Catalyst design relies heavily on electronic metal‐support interactions,but the metal‐support interface with an uncontrollable electronic or coordination environment makes it ***,we outline a promising approach for the rational design of catalysts involving heteroatoms as anchors for Pd nanoparticles for ethanol oxidation reaction(EOR)*** doped B and N atoms from dimethylamine borane(DB)occupy the position of the Ti_(3)C_(2)lattice to anchor the supported Pd *** electrons transfer from the support to B atoms,and then to the metal Pd to form a stable electronic center.A strong electronic interaction can be produced and the d‐band center can be shifted down,driving Pd into the dominant metallic state and making Pd nanoparticles deposit uniformly on the ***‐obtained Pd/DB–Ti_(3)C_(2)exhibits superior durability to its counterpart(∼14.6%retention)with 91.1%retention after 2000 cycles,placing it among the top single metal anodic ***,in situ Raman and density functional theory computations confirm that Pd/DB–Ti_(3)C_(2)is capable of dehydrogenating ethanol at low reaction energies.

关键词： durability electronic interactions ethanol oxidation heteroatom codoping Pd/MXene

The homogenous growth of Co-based coordination compound on graphene nanosheet for high-performance K-organic battery and its reaction mechanism

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Rare Metals 2024年第4期43卷 1622-1634页

作者： Qian-Qian Peng Yi-Ting Wang Shuo Qi Yao Xiao Yong Wang Shuang-Qiang Chen school of Environmental and chemical Engineering Shanghai UniversityShanghai200444China school of Chemistry and Materials Engineering Wenzhou UniversityWenzhou325035China

Metal coordination compounds(MCCs)are gaining popularity for potassium-ion batteries(PIBs)owing to their tuneable structure,multiple reaction sites,low cost and unique ***,they are generally subjected to intrinsic features of the sluggish ionic diffusion coefficient,low electronic conductivity and slow ***,a new MCC material of cobalt-1,3,5-trioxy-2,4,6-triamino-benzo(Co-TB)coordination compound was synthesized and homogenously grown on the surface of graphene nanosheets(GNS),forming a Co-TB@GNS composite with enhanced electronic conductivity and flexible *** from the overall enhanced conductivity,high surface area and abundant activated K-storage sites,Co-TB@GNS electrodes have exhibited superior cycling performance with high reversible capacities(312 mAh·g^(-1)after 100 cycles at 100 mA·g^(-1),224 mAh·g^(-1)after 500 cycles at 1 A·g^(-1))and better rate performances compared with the pure Co-TB compound when served as PIB's ***,multiple in-situ measurement techniques have jointly confirmed that the organic functional groups(C=O,C=N and C=C of benzene rings)and Co^(2+)in Co-TB are the main reversible K-storage sites,including in-situ Fourier transform infrared spectroscopy(FTIR)and X-ray diffraction(XRD),and partial capacity contribution is originated from GNS by the apparent K-storage behavior in the in-situ XRD pattern,proving the possibility of K-storage for metal-organic materials.

关键词： Metal coordination compounds Potassiumion battery Cobalt coordination compound K-storage mechanism

CO_(2) hydrogenation to methanol over the copper promoted In_(2)O_(3) catalyst

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Journal of Energy Chemistry 2024年第6期93卷 135-145,I0004页

作者： Rui Zou Chenyang Shen Kaihang Sun Xinbin Ma Zhuoshi Li Maoshuai Li Chang-Jun Liu school of chemical Engineering and Technology Tianjin UniversityTianjin 300350China Collaborative Innovation Center of chemical Science&Engineering Tianjin UniversityTianjin 300072China

The metal promoted In_(2)O_(3) catalysts for CO_(2) hydrogenation to methanol have attracted wide attention because of their high activity with high methanol ***,there was still no experimental confirmation if copper could be a good promoter for In_(2)O_(3).Herein,the Cu promoted In_(2)O_(3) catalyst was prepared using a deposition-precipitation *** prepared Cu/In_(2)O_(3) catalyst shows significantly higher CO_(2) conversion and space time yield(STY)of methanol,compared to the un-promoted In_(2)O_(3) *** loading of Cu facilitates the activation of both H_(2) and CO_(2) with the interface between the Cu cluster and defective In_(2)O_(3) as the active *** Cu/In_(2)O_(3) catalyst takes the CO hydrogenation pathway for methanol synthesis from CO_(2) *** exhibits a unique size effect on the CO *** temperatures below 250℃,CO adsorption on Cu/In_(2)O_(3) is stronger than that on In_(2)O_(3),causing higher methanol *** increasing temperatu res,the Cu catalyst aggregates,which leads to the formation of weak CO adsorption site and causes a decrease in the methanol *** with other metal promoted In_(2)O_(3) catalysts,it can be concluded that the catalyst with stronger CO adsorption possesses higher methanol selectivity.

关键词： CO_(2)hydrogenation Methanol Cu In_(2)O_(3) CO Selectivity DFT

Methanol steam reforming for hydrogen production driven by an atomically precise Cu catalyst

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Green Energy & Environment 2024年第7期9卷 1079-1084页

作者： Weigang Hu Haoqi Liu Yuankun Zhang Jiawei Ji Guangjun Li Xiao Cai Xu Liu Wen Wu Xu Weiping Ding Yan Zhu school of Chemistry and chemical Engineering Nanjing UniversityNanjing210093China school of Physical Science and Technology Ningbo UniversityNingbo315211China

Plasmon-induced hot-electron transfer from metal nanostructures is being intensely pursed in current photocatalytic research,however it remains elusive whether molecular-like metal clusters with excitonic behavior can be used as light-harvesting materials in solar energy utilization such as photocatalytic methanol steam *** this work,we report an atomically precise Cu_(13)cluster protected by dual ligands of thiolate and phosphine that can be viewed as the assembly of one top Cu atom and three Cu_(4)*** Cu_(13)H_(10)(SR)_(3)(PR’_(3))_(7)(SR=2,4-dichlorobenzenethiol,PR’_(3)=P(4-FC_(6)H_(4))_(3))cluster can give rise to highly efficient light-driven activity for methanol steam reforming toward H_(2)production.

关键词： Nanocluster Photocatalysis Methanol steam reforming Atomically precise Copper catalyst

A review of ultra-high temperature heat-resistant energetic materials

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Defence Technology（防务技术） 2024年第8期38卷 33-57页

作者： Rongzheng Zhang Yuangang Xu Feng Yang Pengcheng Wang Qiuhan Lin Hui Huang Ming Lu school of Chemistry and chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China Institute of chemical Materials China Academy of Engineering PhysicsMianyang 621900China

Heat-resistant energetic materials refer to a type of energetic materials that possess a high melting point,high stability and operational safety. By studying the structures of these energetic materials has showed that the thermal stability can be enhanced by introducing amino groups to form intra/inter-molecular hydrogen bonds, constructing conjugate systems and designing symmetrical structures. This article aims to review the physical and chemical properties of ultra-high temperature heat-resistant energetic compounds and provide valuable theoretical insights for the preparation of ultra-high temperature heatresistant energetic materials. We also analyze the selected 20 heat-resistant energetic materials with decomposition temperatures higher than 350℃, serving as templates for the synthesis of various highperformance heat-resistant energetic materials.

关键词： Heat-resistant energetic materials Organic synthesis Conjugated Hydrogen bond Symmetrical structure Stabilization