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Carbon fiber confined mixed Ni-based crystal phases with interfacial charge redistribution induced by high bond polarity for electrochemical urea-assisted hydrogen generation

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Carbon Energy 2024年第9期6卷 292-305页

作者： Chun Yin Jiaxin Li Shuli Wang Huan Wen Fulin Yang Ligang Feng school of chemistry and Chemical engineering Yangzhou UniversityYangzhouChina Guangxi Key Laboratory of Electrochemical Energy Materials School of Chemistry and Chemical EngineeringGuangxi UniversityNanningChina

Interfacial electronic structure modulation of nickel-based electrocata-lysts is significant in boosting energy-conversion-relevant urea oxidation reaction(UOR).Herein,porous carbon nanofibers confined mixed Ni-based crystal phases of Ni_(2)P and NiF_(2) are developed via fluorination and phosphorization of Ni coated carbon nanofiber(Ni_(2)P/NiF_(2)/PCNF),which possess sufficient mesoporous and optimized Gibbs adsorption free energy by mixed phase-induced charge *** novel system further reduces the reaction energy barrier and improves the reaction activity by addressing the challenges of low intrinsic activity,difficulty in active site formation,and insufficient synergism.A considerably high current density of 254.29 mA cm^(-2) is reached at 1.54 V versus reversible hydrogen electrode on a glass carbon electrode,and the cell voltage requires 1.39 V to get 10 mA cm^(-2) in hydrogen generation,with very good stability,about 190 mV less than that of the traditional water *** facile active phase formation and high charge transfer ability induced by asymmetric charge redistribution are found in the interface,where the urea molecules tend to bond with Ni atoms on the surface of heterojunction,and the rate-determining step is changed from CO_(2) desorption to the fourth H-atom *** work reveals a novel catalyst system by interfacial charge redistribution induced by high bond polarity for energy-relevant catalysis reactions.

关键词： carbon fiber nickel fluoride nickel phosphide urea oxidation water electrolysis

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Distinct effect of preparation methods on reaction efficiency of Mn-Ce/Al_(2)O_(3) catalysts in low-temperature NH_(3)-SCR

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Journal of Rare Earths 2024年第10期42卷 1865-1872页

作者： Shijie Hao Yandi Cai Wei Wei Yanan Lv Jjiawei Ji Wei Tan Jingfang Sun Liwei Jia Changjin Tang Lin Dong State Key Laboratory of Pollution Control and Resource Reuse School of Environmentjiangsu Key Laboratory of Vehicle Emissions ControlCenter of Modern AnalysisKey Laboratory of Mesoscopic Chemistry of MOESchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Wuxi Weifu environmental Catalysts Co. LtdWuxi214028China school of environment Nanjing Normal UniversityNanjing210023China

In this study,a series of Mn-Ce/Al_(2)O_(3) catalysts was prepared by different methods of depositionprecipitation(MnCeAl-DP),impregnation(MnCeAl-IM) and citric acid(MnCeAl-CA),and the distinct effect of preparation methods on NO_x removal performance at low temperature was *** show that MnCeAl-DP exhibits not only the best activity but also the highest resistance against SO_(2)/H_(2)*** the assistance of comprehensive characterizations from scanning electron microscopy(SEM),Brunauer-Emmett-Teller(BET),X-ray diffraction(XRD),H_(2)-temperature programmed reduction(H_(2)-TPR),NH_(3)-te mperature programmed deso rption(NH_(3)-TPD),and X-ray photoelectron spectroscopy(XPS),it is revealed that the MnCeAl-DP sample owns admired features of large surface area and pore volume,enriched Mn^(4+) and chemisorbed oxygen species originating from enhanced interaction between MnO_x and CeO_(2),as well as improved adsorption capacity to NH_3 and *** these factors contribute to activity *** in-situ DRIFTS studies reveal that the improvement of NH_(3)-SCR performance over MnCeAI-DP is related to the formation of abundant nitrate species,which is beneficial to the "NH_(4)NO_(3)" reaction pathway and thus enhances low-temperature activity.

关键词： Mn-Ce/Al_(2)O_(3)catalysts NH_(3)-SCR Low temperature NH_(4)NO_(3) Fast SCR Rare earths

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One-step growth of ultrathin CoSe_(2)nanobelts on N-doped MXene nanosheets for dendrite-inhibited and kinetic-accelerated lithium-sulfur chemistry

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Science Bulletin 2024年第13期69卷 2059-2070页

作者： Chuanliang Wei Zhengran Wang Peng Wang Xinlu Zhang Xuguang An Jinkui Feng Baojuan Xi Shenglin Xiong school of chemistry and Chemical engineering School of Materials Science and EngineeringShandong UniversityJinan 250100China school of Mechanical engineering Chengdu UniversityChengdu 610106China

The practical application of lithium–sulfur(Li–S)batteries is inhibited by the shuttle effect of lithium polysulfides(LiPSs)and slow polysulfide redox kinetics on the S cathode as well as the uncontrollable growth of dendrites on the Li metal ***,both cathode and anode sides must be considered when modifying LiS ***,two-dimensional(2D)ultrathin CoSe_(2)nanobelts are in situ grown on 2D N-doped MXene nanosheets(CoSe_(2)@N-MXene)via one-step solvothermal process for the first *** to its unique 2D/2D structure,CoSe_(2)@N-MXene can be processed to crumpled nanosheets by freeze-drying and flexible and freestanding films by vacuum *** crumpled CoSe_(2)@NMXene nanosheets with abundant active sites and inner spaces can act as S hosts to accelerate polysulfide redox kinetics and suppress the shuttle effect of LiPSs owing to their strong adsorption ability and catalytic conversion effect with ***,the CoSe_(2)@N-MXene film(CoSe_(2)@NMF)can act as a current collector to promote uniform Li deposition because it contains lithiophilic CoSe_(2)and N *** the systematic effect of CoSe_(2)@N-MXene on S cathode and Li metal anode,the electrochemical and safety performance of Li–S batteries are ***_(2)@NMF also shows excellent storage performances in flexible energy storage devices.

关键词： Ultrathin CoSe_(2)nanobelts N-doped MXene nanosheets In situ growth Flexible MXene-based films Li-S batteries

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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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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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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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Metal-organic frameworks on 3D interconnected macroporous sponge foams for large-scale water decontamination:A mini review

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Chinese Chemical Letters 2024年第5期35卷 77-84页

作者： Xiao-Hong Yi Chong-Chen Wang Beijing Key Laboratory of Functional Materials for Building Structure and environment Remediation School of Environment and Energy EngineeringBeijing University of Civil Engineering and ArchitectureBeijing 100044China

Water pollution caused by global population growth,urban expansion and industrialization development is one of the urgent issues that need to be addressed in the 21st *** to now,it was challenging for metal-organic frameworks(MOFs)to be used in the actual water treatment due to that the powder MOFs suffered from difficult reuse,poor water stability and easy *** is an effective strategy to immobilize MOFs powder onto porous sponge foam carriers for accomplishing large flux,facile recycling,easy processing water treatment *** this review article,the fabrication approaches and applications of different MOFs/sponge composites were highlighted,in which the fluorescence detection of pollutants,adsorption and separation of pollutants,catalytic reduction and oxidation of pollutants were ***,the future challenges and opportunities of MOF/sponge for water treatment are proposed,aiming to provide in-depth guidance for the future design and manufacture of the immobilized MOFs onto sponge foams.

关键词： Metal-organic frameworks Sponge foam Water decontamination Adsorption Catalysis

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Production of the C/TiO_(2)composite with a high-performance electrochemical property from titanium-rich sludge via in-situ C coating

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Journal of environmental Sciences 2024年第3期137卷 131-143页

作者： Hualong Wu Yanxia Zhao Jiexi Wang Xiaoyan Li Kaimin Shih Xuguang Li Wei Liu school of Water Conservancy and environment University of JinanJinan 250022China State Key Lab of Physical chemistry of Solid Surface Collaborative Innovation Center of Chemistry for Energy MaterialsCollege of MaterialsXiamen UniversityXiamen 361005China school of Metallurgy and environment Central South UniversityChangsha 410083China Department of Civil engineering The University of Hong KongPokfulamHong KongChina Institute of environment and Ecology Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China

Resource recycling from waste-water and sludge is an important part of the 14th Five-Year Plan in *** emerging titanium-based coagulants have drawn growing attentions due to their strong coagulation capability in water purification and value-added Ti-loaded sludge *** and recovery of the high value-added sludge into functional nanomaterials is highly significant for both sludge reduction and environmental *** present study was carried out to investigate the recycle of the coagulated Ti-loaded sludge to produce functional C/TiO_(2)composites as the anode materials for lithium-ion batteries(LIBs).It is the first time that the application of the Ti-loaded wastewater sludge derived C/TiO_(2)was evaluated for *** experimental results showed that the carbon coating through in-situ carbonization of the sludge produced the C/TiO_(2)composites with a high specific surface area,stable structural integrity,and excellent electrochemical properties that would facilitate Li+diffusion in long-term LIBs *** C/TiO_(2)composites calcinated from the polytitanium sulfate-coagulated sludge at 800℃(N_(2))exhibited the best electrochemical performance during the cycling tests(601 m Ah/g at 100 m A/g after 200 cycles).The research work demonstrates the promising prospect of the recycle and value-added utilization of the Ti-loaded sludge in the production of high-performance C/TiO_(2)composites for energy storage *** study provides a new way for the management and reuse of Ti-loaded waste-sludge.

关键词： Sludge recovery Ti-loaded sludge In-situ coating Lithium-ion battery

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A healable, mechanically robust and ultrastretchable ionic conductive elastomer for durably wearable sensor

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Nano Research 2024年第4期17卷 3369-3378页

作者： Guoxian Zhang Chunmei Li JiaoJun Tan Mingqi Wang Yafeng Ren Feijie Ge Qiuyu Zhang Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi'an 710072China College of Bioresources Chemical and Materials engineering National Demonstration Center for Experimental Light Chemistry Engineering EducationShaanxi University of Science&TechnologyXi’an 710021China

The ionic conductive elastomers show great promise in multifunctional wearable electronics,but they currently suffer from liquid leakage/evaporation or mechanical *** ionic conductive elastomers integrating non-volatility,mechanical robustness,superior ionic conductivity,and ultra-stretchability remains urgent and ***,we developed a healable,robust,and conductive elastomer via impregnating free ionic liquids(ILs)into the ILs-multigrafted poly(urethane-urea)(PUU)elastomer networks.A crucial strategy in the molecular design is that imidazolium cations are largely introduced by double-modification of PUU and centipede-like structures are obtained,which can lock the impregnated ILs through strong ionic *** this system,the PUU matrix contributes outstanding mechanical properties,while the hydrogen bonds and ionic interactions endow the elastomer with self-healing ability,conductivity,as well as non-volatility and *** fabricated ionic conductive elastomers show good conductivity(3.8×10^(-6) S·cm^(-1)),high mechanical properties,including tensile stress(4.64 MPa),elongation(1470%),and excellent healing ability(repairing efficiency of 90%after healing at room temperature for 12 h).Significantly,the conductive elastomers have excellent antifatigue properties,and demonstrate a highly reproducible response after 1000 uninterrupted extension-release *** work provides a promising strategy to prepare ionic conductive elastomers with excellent mechanical properties and stable sensing capacity,and further promote the development of mechanically adaptable intelligent sensors.

关键词： ionic conductive elastomers poly(urethane-urea)(PUU) ionic interactions centipede-like self-healing

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