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Self-separation ionic liquid catalyst for the highly effective conversion of H2S by α,β-unsaturated carboxylate esters under mild conditions

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Green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu Key Laboratory of Mesoscopic chemistry of MOE School of Chemistry and Chemical Engineering Nanjing University The Institute of Green chemistry and engineering School of Chemistry and Chemical Engineering Nanjing University

The deep-processing utility of pure hydrogen sulfide （H2S） is a significant direction in natural gas chemical ***,a brand-new strategy of H2S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids （ILs） as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H2S to a,β-unsaturated carboxylate ***,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H2S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H2S utilization,which will guide its application on an industrial scale.

关键词： Ionic liquid Cascade reaction Self-separation H 2 S conversion Catalysis

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Preparation of bifunctional electrocatalyst by recycling heavy metal ions from wastewater using EDTAD-functionalized MOF as highly efficient adsorbent

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Rare Metals 2024年第10期43卷 5105-5116页

作者： Yue Qian Pei-Xue Fu Rui-Ze Yin Han-Ni Yang Si-Yang Li Wei-Wei Xiong Fen-Fen Zheng Jun-Hao Zhang Ai-Hua Yuan Huan Pang school of Environmental and chemical engineering Jiangsu University of Science and Technology school of chemistry and chemical engineering Yangzhou University

The recovery and subsequent reuse of heavy metal ions from industrial wastewater are crucial for promoting sustainable development,but they also presen significant *** this article,ethylenediaminetetraacetic dianhydride （EDTAD）,which possesses strong metal chelating ability,is covalently attached to MIL-101-NH2（Fe）,resulting in a significant improvement in the removal rate of heavy metal ions in ***,the recovered waste metal ions are transformed into high-performance FeNi3/NiFe2O4@NC dual-functional oxygen evolution reaction （OER） and oxygen reduction reaction （ORR） ***,FeNi3/NiFe2O4@NC exhibits outstanding OER performance,with only a264 mV overpotential at 10 mA·*** functiona theory （DFT） calculations reveal that the synergistic effect of the FeNi3/NiFe2O4@NC heterostructure can enhance conductivity,optimize the free energy of*to OH*during OER reaction,and promote catalytic *** work not only improves the removal rate of heavy metal ions but also obtains high-performance catalysts,while providing a new approach for the treatment and secondary utilization of heavy metal ion wastewater as well as the preparation of low-cost catalysts.

关键词： Bifunctional electrocatalyst Covalently modified MOF Ethylenediaminetetraacetic dianhydride Heavy metals

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Silvery fullerene in Ag102 nanosaucer

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National Science Review 2024年第7期11卷 158-167页

作者： Zhi Wang Yuchen Wang Chengkai Zhang Yan-Jie Zhu Ke-Peng Song Christine M.Aikens Chen-Ho Tung Di Sun school of chemistry and chemical engineering Shandong University Department of chemistry Kansas State University

Despite the discovery of a series of fullerenes and a handful of noncarbon clusters with the typical topology of Ih-C60, the smallest fullerene with a large degree of curvature, C20, and its other-element counterparts are difficult to isolate experimentally. In coinage metal nanoclusters（NCs）, the first all-gold fullerene, Au32, was discovered after a long-lasting pursuit, but the isolation of similar silvery fullerene structures is still challenging. Herein, we report a flying saucer-shaped 102-nuclei silver NC（Ag102） with a silvery fullerene kernel of Ag32, which is embraced by a robust cyclic anionic passivation layer of（KPO4）10. This Ag32kernel can be viewed as a non-centered icosahedron Ag12encaged into a dodecahedron Ag20, forming the silvery fullerene of Ag12@Ag20. The anionic layer（KPO4）10is located at the interlayer between the Ag32kernel and Ag70shell, passivating the Ag32silvery fullerene and templating the Ag70shell. The ~tBuPhS-and CF3COO-ligands on the silver shell show a regioselective arrangement with the 60 ~tBuPhS-ligands as expanders covering the upper and lower of the flying saucer and 10 CF3COO-as terminators neatly encircling the edges of the structure. In addition, Ag102 shows excellent photothermal conversion efficiency（η） from the visible to near-infrared region（η = 67.1% ± 0.9% at 450 nm, 60.9% ± 0.9% at 660 nm and 50.2% ± 0.5% at 808 nm）, rendering it a promising material for photothermal converters and potential application in remote laser ignition. This work not only captures silver kernels with the topology of the smallest fullerene C20, but also provides a pathway for incorporating alkali metal（M） into coinage metal NCs via M-oxoanions.

关键词： silvery fullerene >Ag102 nanosaucer cyclic anionic passivation layer photothermal conversion DFT calculation

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Precision design of Ti sites for unprecedented catalytic performance

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National Science Review 2024年第7期11卷 67-68页

作者： Haoquan Zheng Shunai Che Key Laboratory of Applied Surface and Colloid chemistry Ministry of Education School of Chemistry and Chemical Engineering Shaanxi Normal University school of chemistry and chemical engineering Shanghai Jiao Tong University

In 1983, Taramasso et al. incorporated titanium(Ti) into porous silica frameworks to endow Ti sites with catalytic oxidation ability [1]. Nowadays, catalytic oxidation reactions using titanium silicate materials have ...

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The Al_(2)O_(3)and Mn/Al_(2)O_(3)sorbents highly utilized in destructive sorption of NF_(3)

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Chinese Journal of chemical engineering 2024年第1期65卷 54-62页

作者： Yanfei Pan Hejian Li Li Zheng Xiufeng Xu school of chemistry and chemical engineering Yantai UniversityYantai 264005China

NF_(3)is commonly used as an etching and cleaning gas in semiconductor industry,however it is a strongly greenhouse ***,the destruction of disposal NF_(3)is an urgent task to migrate the greenhouse *** the technologies for NF_(3)abatement,the destructive sorption of NF_(3)over metal oxides sorbents is an effective ***,the search for a highly reactive and utilized sorbent for NF_(3)destruction is in great *** this work,AlOOH supported on carbon-sphere(AlOOH/CS)as precursors were synthesized hydrothermally and heat-treated to prepare the Al_(2)O_(3)*** influence of AlOOH/CS hydrothermal temperatures on the reactivity of derived Al_(2)O_(3)sorbents for NF_(3)destruction was investigated,and it is shown that the Al2O3 from AlOOH/CS hydro-thermalized at 120℃is superior to ***,the optimized Al_(2)O_(3)was covered by Mn(OH)x to prepare Mn/Al_(2)O_(3)sorbents via changing hydrothermal temperatures and Mn *** results show that the Mn/Al_(2)O_(3)sorbents are more utilized than bare Al_(2)O_(3)in NF_(3)destructive sorption due to the promotional effect of Mn_(2)O_(3)as surface layer on the fluorination of Al_(2)O_(3)as substrate,especially the optimal 5%Mn/Al2O3(160℃)exhibits a utilization percentage as high as 90.4%,and remarkably exceeds all the sorbents reported so *** findings are beneficial to develop more efficient sorbents for the destruction of NF_(3).

关键词： Greenhouse gas NF_(3)destructive sorption Sorbents Al_(2)O_(3) Mn/Al_(2)O_(3) Reactivity

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Guest-adaptive chiral coassembly of a conformationally locked host into supramolecular boxes and ladders through arene-perfluoroarene force

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Science China chemistry 2024年第10期67卷 3482-3492页

作者： Weilong Ma Xinyi Li Aiyou Hao Pengyao Xing school of chemistry and chemical engineering Shandong UniversityJinan 250100China

Unveiling the role of weak non-covalent forces in chiral self-assembly is pivotal in the design and fabrication of functional chiroptical *** nature of arene-perfluoroarene(AP)force is the electrostatic attraction betweenπ-hole andπplanes of perfluoroarenes and polyaromatic hydrocarbons(PAHs),which is emerging in constructing supramolecular motifs and coassembled optical *** this work,we reveal the potential of AP forces in building diversified levels of chiral coassemblies adaptive to the geometries of *** naphthalene-F8was covalently conjugated with a chiral amine,which folded into a semi-rectangular geometry via two intramolecular F···H *** of naphthalene,anthracene,pyrene,carbazole,perylene and benzoperylene were introduced to afford coassemblies in the crystalline state.X-ray structures suggest the formation of supramolecular boxes that encapsulate the PAHs with a 2:1 stoichiometric ratio,as well as the formation of consecutive layered ladders with a 1:1 stoichiometric *** preference is adaptive to the geometries of PAHs,and experimental and computational results evidenced the ladder structures possess strong binding *** this top,the selective chiral recognition in the mixtures of PAHs was realized,which shows promising applications in the separation of PAHs and rational design of crystalline chiroptical materials.

关键词： arene-perfluoroarene force coassembly supramolecular chirality selectivity

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Phase and chemical state tuning of FeNi oxides for oxygen evolution reaction

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Science China chemistry 2024年第8期67卷 2755-2766页

作者： Jiawei Wu Zhouyang Ma Lice Yu Shuli Wang Fulin Yang Ligang Feng school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China

Advancing and deploying the Fe Ni-based catalyst,the state-of-the-art pre-electrocatalysts,for oxygen evolution reactions(OER)still suffer from unclear chemical state correlation to the catalytic ability,as evidenced by the variedly reported performance for the different Fe Ni ***,we contributed the phase and redox chemical states tuning of Fe Ni oxides by the surface microenvironment regulation for the OER catalysis that was realized by the urea-assisted pyrolysis and molybdenum-doping technique by integrating molybdenum into the iron–nickel metal-organic *** by the complicated and compromised atmosphere,namely,the oxidation state driven by the Mo doping and reduction ability induced by the urea-assisted pyrolysis,could transfer confined Fe Ni oxides to hybrid phases of Fe_(2)O_(3)and FeNi_(3)alloy,and the resultant compromised chemical states by the charge redistribution imparted very high electrocatalytic performance for OER compared with the control *** insitu Raman spectroscopy and post-XPS analysis confirmed the facile Fe/Ni oxyhydroxide active phase formation resulting from the proper phase and chemical states,and theoretical analysis disclosed the microenvironment regulation resulting in the charge redistribution forming the electron accumulation and depletion sites to accelerate the oxygen-species to oxyhydroxide-species transformation and enhance the electronic state density near the Fermi level by significantly reducing the energy *** work not only showed the importance of surface chemical state tunning that can basically answer the varied performance of Fe Ni catalysts but also revealed an effective approach for fine-tuning their catalytic properties.

关键词： oxygen evolution reaction FeNi-based catalysts urea pyrolysis chemical states charge redistribution

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Exceptional Performance of 3D Additive Manufactured NiFe Phosphite Oxyhydroxide Hollow Tubular Lattice Plastic Electrode for Large-Current-Density Water Oxidization

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Energy & Environmental Materials 2024年第6期7卷 262-273页

作者： Liping Ding Lin Zhang Gaoyuan Li Shuyan Chen Han Yan Haibiao Tu Jianmin Su Qi Li Yanfeng Tang Yanqing Wang school of chemistry and chemical engineering Nantong UniversityNantong 226007China

In this article,we report a 3D NiFe phosphite oxyhydroxide plastic electrode using high-resolution digital light processing(DLP)3D-printing technology via induced chemical deposition *** as-prepared 3D plastic electrode exhibits no template requirement,freedom design,low-cost,robust,anticorrosion,lightweight,and micro-nano porous *** can be drawn to the conclusion that highly oriented open-porous 3D geometry structure will be beneficial for improving surface catalytic active area,wetting performance,and reaction–diffusion dynamics of plastic electrodes for oxygen evolution reaction(OER)catalysis *** functional theory(DFT)calculation interprets the origin of high activity of NiFe(PO_(3))O(OH)and demonstrates that the implantation of the–PO_(3)can effectively bind the 3d orbital of Ni in NiFe(PO_(3))O(OH),lead to the weak adsorption of intermediate,make electron more active to improve the conductivity,thereby lowing the transform free energy of*O to**** water oxidization performance of as-prepared 3D NiFe(PO_(3))O(OH)hollow tubular(HT)lattice plastic electrode has almost reached the state-of-the-art level compared with the as-reported large-current-density catalysts or 3D additive manufactured plastic/metal-based electrodes,especially for high current OER *** work breaks through the bottleneck that plagues the performance improvement of low-cost high-current electrodes.

关键词： 3D plastic electrode 3D printing induced chemical deposition largecurrent-density water oxidization NiFe phosphite oxyhydroxide

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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 University school of Physical Science and Technology Ningbo University

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 Cu13cluster protected by dual ligands of thiolate and phosphine that can be viewed as the assembly of one top Cu atom and three *** Cu13H10（SR）3（PR’3）7(SR=2,4-dichlorobenzenethiol,PR’3=P（4-FC6H4）3) cluster can give rise to highly efficient light-driven activity for methanol steam reforming toward H2production.

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

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Emerging perovskite materials for supercapacitors:Structure,synthesis,modification,advanced characterization,theoretical calculation and electrochemical performance

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Journal of Energy chemistry 2024年第2期89卷 41-70,I0003页

作者： Yuehua Qian Qingqing Ruan Mengda Xue Lingyun Chen Department of Applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China

As a new generation electrode materials for energy storage,perovskites have attracted wide attention because of their unique crystal structure,reversible active sites,rich oxygen vacancies,and good *** this review,the design and engineering progress of perovskite materials for supercapacitors(SCs)in recent years is ***,the review will focus on four types of perovskites,perovskite oxides,halide perovskites,fluoride perovskites,and multi-perovskites,within the context of their intrinsic structure and corresponding electrochemical performance.A series of experimental variables,such as synthesis,crystal structure,and electrochemical reaction mechanism,will be carefully analyzed by combining various advanced characterization techniques and theoretical *** applications of these materials as electrodes are then featured for various ***,we look forward to the prospects and challenges of perovskite-type SCs electrodes,as well as the future research direction.

关键词： Perovskite Modification engineering Oxygen vacancy Theoretical calculation methodology Supercapacitor

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