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Triple the steady-state reaction rate by decorating the In_(2)O_(3)surface with SiO_(x)for CO_(2)hydrogenation

Journal of Energy Chemistry 2024年第8期95卷 96-105,I0003页

作者： Hao Wang Chun Yang Xiaoyan Yu Mingrui Wang Runze Yang Xiaowa Nie Ben Hang Yin Alex C.K.Yip Chunshan Song Guanghui Zhang Xinwen Guo State Key Laboratory of Fine Chemicals Frontier Science Center for Smart MaterialsPSU-DUT Joint Center for Energy ResearchSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Department of Chemistry the Chinese University of Hong KongHong Kong 999077China Paihau-Robinson Research Institute the MacDiarmid Institute for Advanced Materials and NanotechnologyVictoria University of WellingtonWellington 6012New Zealand Department of Chemical and Process Engineering The University of CanterburyChristchurch 8041New Zealand

Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction *** on the comprehension of the dynamic evolution,this study presents an efficient strategy to alleviate the agglomeration of In_(2)O_(3)nanoparticles by the surface decoration with highly dispersed silica species(SiO_(x)).Various structural characterizations combined with density functional theory calculations demonstrated that the sintering resulted from the over-reduction,while the enhanced stability originated from the anchoring effect of highly stable In-OSi bonds,which hinders the substantial formation of metallic In(In^(0))and the subsequent agglomeration.0.6Si/In_(2)O_(3)exhibited CO_(2)conversion rate of10.0 mmol g^(-1)h^(-1)at steady state vs.3.5 mmol g^(-1)h^(-1)on In_(2)O_(3)in CO_(2)*** steady-state activity was also achieved on Pd-modified *** to the traditional Pd/In_(2)O_(3)catalyst,the methanol production rate of Pd catalyst supported on 0.6Si/In_(2)O_(3)was enhanced by 23%,showing the potential of In_(2)O_(3)modified by SiO_(x)in serving as a platform *** work provides a promising method to design new In_(2)O_(3)-based catalysts with improved activity and stability in CO_(2)hydrogenation.

关键词： CO_(2)hydrogenation In_(2)O_(3)sintering Dynamic structural evolution Surface SiO_(x)modification DFT simulations

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Hydrogen-based direct reduction of industrial iron ore pellets:Statistically designed experiments and computational simulation

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International Journal of Minerals,Metallurgy and Materials 2022年第10期29卷 1908-1921页

作者： Patrícia Metolina Tiago Ramos Ribeiro Roberto Guardani Chemical Systems Engineering Center Department of Chemical EngineeringUniversity of São PauloSão Paulo 05508-900Brazil Metallurgical Process Laboratory Institute of Technological ResearchSão Paulo 05508-901Brazil

As part of efforts to reduce anthropogenic CO_(2) emissions by the steelmaking industry,this study investigated the direct reduction of industrially produced hematite pellets with H_(2) using the Doehlert experimental design to evaluate the effect of pellet diameter(10.5-16.5 mm),porosity(0.36-0.44),and temperature(600-1200℃).A strong interactive effect between temperature and pellet size was observed,indicating that these variables cannot be considered *** increase in temperature and decrease in pellet size considerably favor the reduction rate,while porosity did not show a relevant *** change in pellet size during the reduction was negligible,except at elevated temperatures due to crack formation.A considerable decrease in mechanical strength at high temperatures suggests a maximum process operating temperature of 900℃.Good predictive capacity was achieved using the modified grain model to simulate the three consecutive non-catalytic gas-solid reactions,considering different pellet sizes and porosities,changes during the reaction from 800 to 900℃.However,for other temperatures,different mechanisms of structural modifications must be considered in the *** results represent significant contributions to the development of ore pellets for CO_(2)-free steelmaking technology.

关键词： hydrogen use non-catalytic gas-solid reaction grain model porous hematite pellet CO_(2)emissions reduction Doehlert experimental design

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Transferable,highly crystalline covellite membrane for multifunctional thermoelectric systems

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InfoMat 2024年第11期6卷 66-80页

作者： Myungwoo Choi Geonhee Lee Yea-Lee Lee Hyejeong Lee Jin-Hoon Yang Hanhwi Jang Hyeonseok Han MinSoung Kang Seonggwang Yoo A-Rang Jang Yong Suk Oh Inkyu Park Min-Wook Oh Hosun Shin Seokwoo Jeon Jeong-O Lee Donghwi Cho Department of Materials Science and Engineering Korea UniversitySeoulRepublic of Korea Thin Film Materials Research Center Korea Research Institute of Chemical TechnologyDaejeonRepublic of Korea Chemical Data-Driven Research Center Korea Research Institute of Chemical TechnologyDaejeonRepublic of Korea Division of Chemical and Material Metrology Korea Research Institute of Standards and ScienceDaejeonRepublic of Korea Department of Materials Science and Engineering Korea Advanced Institute of Science and TechnologyDaejeonRepublic of Korea Department of Mechanical Engineering Korea Advanced Institute of Science and TechnologyDaejeonRepublic of Korea Therapeutics&Biotechnology Division Drug Discovery Platform Research CenterKorea Research Institute of Chemical TechnologyDaejeonRepublic of Korea Querry Simpson Institute for Bioelectronics Northwestern UniversityEvanstonIllinoisUSA Division of Electrical Electronic and Control EngineeringKongju National UniversityCheonanRepublic of Korea Department of Mechanical Engineering Changwon National UniversityChangwonRepublic of Korea Department of Materials Science and Engineering Hanbat National UniversityDaejeonRepublic of Korea Advanced Materials and Chemical Engineering University of Science and TechnologyDaejeonRepublic of Korea

Emerging freestanding membrane technologies,especially using inorganic thermoelectric materials,demonstrate the potential for advanced thermoelectric ***,using rare and toxic elements during material processing must be ***,we present a scalable method for synthesizing highly crystalline CuS membranes for thermoelectric *** sulfurizing crystalline Cu,we produce a highly percolated and easily transferable network of submicron CuS *** CuS membrane effectively separates thermal and electrical properties to achieve a power factor of 0.50 mW m^(-1) K^(-2) and thermal conductivity of 0.37 W m^(-1) K^(-1) at 650 K(estimated value).This yields a record-high dimensionless figure-of-merit of 0.91 at 650 K(estimated value)for ***,integrating 12 CuS devices into a module resulted in a power generation of4μW atΔT of 40 K despite using a straightforward configuration with only p-type ***,based on the temperature-dependent electrical characteristics of CuS,we develop a wearable temperature sensor with antibacterial properties.

关键词： copper sulfide flexible thermoelectric generator multifunctional thermoelectric systems sulfurization thermoelectric membrane

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Carbonitride MXene Ti_(3)CN(OH)_(x)@MoS_(2)hybrids as efficient electrocatalyst for enhanced hydrogen evolution

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Nano research 2023年第4期16卷 4656-4663页

作者： Jizhou Jiang Fangyi Li Saishuai Bai Yongjing Wang Kun Xiang Haitao Wang Jing Zou Jyh-Ping Hsu School of Environmental Ecology and Biological Engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Department of Chemical Engineering “National Taiwan University”Taipei 10617

Renewable energy powered electrocatalytic water splitting is a promising strategy for hydrogen generation,and the design and development of high-efficiency and earth-abundant electrocatalysts for hydrogen evolution reaction(HER)are highly ***,MoS2 nanoflowers decorated two-dimensional carbonitride-based MXene Ti3CN(OH)x hybrids have been constructed by etching and post-hydrothermal *** electrochemical performance of the as-obtained Ti_(3)CN(OH)_(x)@MoS_(2)hybrids having a quasi core-shell structure is fascinating:An overpotential of 120 mV and a Tafel slope of 64 mV∙dec^(−1)can be delivered at a current density of 10 mA∙cm^(−2).And after 3,000 cyclic voltammetry cycles,it can be seen that there is no apparent *** the experimental results and density functional theory(DFT)calculations indicate that the synergetic effects between Ti_(3)CN(OH)x and MoS_(2)are responsible for the robust electrochemical HER *** electrons of-OH group in Ti_(3)CN(OH)x are transferred to MoS_(2),making the adsorption energy of the composite for H almost *** metallic Ti_(3)CN(OH)x is also beneficial to the fast charge transfer *** construction of MXene-based hybrids with optimal electronic structure and unique morphology tailored to the applications can be further used in other promising energy storage and conversion devices.

关键词： Ti_(3)CN(OH)x MoS_(2) hydrogen evolution reaction density functional theory(DFT)calculations

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Well-oriented magnesium hydroxide nanoplatelets coating with high corrosion resistance and osteogenesis on magnesium alloy

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Journal of Magnesium and Alloys 2024年第8期12卷 3292-3307页

作者： Ya Shu Feng Peng Zhi-Hui Xie Qiwen Yong Liang Wu Juning Xie Mei Li Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong637002China Medical Research Institute Department of OrthopedicsGuangdong Provincial People’s Hospital(Guangdong Academy of Medical Sciences)Southern Medical UniversityGuangzhou 510080China College of Materials Science and Engineering/National Engineering Research Center for Magnesium Alloys Chongqing UniversityChongqing 400044China

Magnesium alloys are nontoxic and promising as orthopedic metallic implants,but preparing a biocompatible Mg(OH)_(2)layer with high corrosion protection ability remains *** is generally believed that the Mg(OH)_(2)layer,especially that formed in a natural condition,cannot provide desirable corrosion resistance in the community of corrosion and ***,several Mg(OH)_(2)coatings were prepared by changing the pH values of sodium hydroxide *** coatings were composed of innumerable nanoplatelets with different orientations and showed distinguished capability in corrosion *** nanoplatelets were well-oriented with their ab-planes parallel to,instead of perpendicular to,the magnesium alloy surface by raising the pH value to *** specific orientation resulted in the optimal coating showing long-term corrosion protection in both in vitro and in vivo environments and good osteogenic *** finds manifest that the environment-friendly Mg(OH)_(2)coating can also provide comparable and better corrosion protection than many traditional chemical conversion films(such as phosphate,and fluoride).

关键词： Magnesium alloy Corrosion Coating Magnesium hydroxide Biomaterials

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Ultrasonic enhancement of persulfate oxidation system governs emerging pollutants decontamination

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Green Energy & Environment 2024年第11期9卷 1666-1678页

作者： Yanpan Li Yanbo Zhou Yi Zhou National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical ProcessEast China University of Science and Technology130 Meilong RoadShanghai200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and Technology130 Meilong RoadShanghai200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

Emerging contaminants (ECs) are widely present in aquatic environments, posing potential risks to both ecosystems and human health. Theultrasound-assisted persulfate oxidation process has attracted considerable attention in the degradation of ECs due to its ability to generate bothsulfate radicals and cavitation effects, enhancing degradation effects. In this paper, the principle of ultrasonic synergistic Fenton-like oxidationsystem for degrading organic pollutants was reviewed, divided into homogeneous system, non-homogeneous system, and single-atom system toexplore the synergistic effect of ultrasound-enhanced persulfate technology in three aspects, and the effects of environmental factors such asultrasonic frequency and power, system pH, temperature, and initial oxidant concentration on the system's decontamination performance werediscussed. Finally, future research on ultrasonically activated persulfate technology is summarized and prospected.

关键词： Ultrasound Persulfate Emerging contaminants Reaction mechanism Synergistic effects

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Screening techniques as a preliminary diagnostic tool for advanced oxidative processes on a laboratory scale

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Frontiers of chemical Science and engineering 2025年第2期19卷 81-91页

作者： Larissa Pinheiro de Souza Flávio Olimpio Sanches-Neto Júlio César de Oliveira Ribeiro Bruno Ramos Valter H.Carvalho-Silva Antonio Carlos Silva Costa Teixeira Research Group in Advanced Oxidation Processes(AdOx) Department of Chemical EngineeringPolytechnic SchoolUniversity of São PauloSão Paulo 05508-010Brazil Modeling of Physical and Chemical Transformations Division Theoretical and Structural Chemistry GroupResearch and Postgraduate CenterGoiás State UniversityAnápolis 75132-903Brazil Federal Institute of Education Science and Technology of GoiásValparaíso de Goiás 72876-601Brazil Department of Chemical Engineering FEI UniversitySão Paulo 09850-901Brazil Chemistry Institute Federal University of GoiásGoiânia 74690-900Brazil

This study introduces an innovative screening approach to evaluate advanced oxidation processes (AOPs) as a preliminary diagnostic tool for degrading emerging contaminants (EC). It includes the design, prototyping, and cost-benefit analysis of circular photochemical reactors with flat and spiral internal geometries. Three-dimensional (3D) printing was used for reactor prototyping, providing flexibility and economy, and this stage was assisted by the hydrodynamic analysis of the prototypes based on residence time distribution (RTD) and macromixing models. The research evaluates the degradation of a model contaminant of emerging concern, fluoxetine (FLX) hydrochloride, using the solar/persulfate (PS) process in two water matrices (i.e., ultrapure water and sewage treatment plant effluent) to optimize reactor performance. The study also proposes primary theoretical pathways for fluoxetine degradation involving hydroxyl and sulfate radicals, as well as predicting the toxicity of the parent compound and its primary metabolites using quantitative structure-activity relationship (QSAR) models. The spiral reactor exhibits improved hydrodynamic behavior, closely resembling continuous stirred and plug flow reactors in series. Despite a slightly lower specific degradation rate in real wastewater, the solar/PS process remains effective for both matrices. By-products generated via the sulfate radical pathway are expected to be less toxic than those formed by hydroxyl radicals (HO·) attack.

关键词： emerging contaminants advanced oxidation process three-dimensional printed reactor quantum chemical calculations toxicity

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Depositing the PtNi nanoparticles on niobium oxide to enhance the activity and CO-tolerance for alkaline methanol electrooxidation

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Chinese Journal of Structural Chemistry 2023年第11期42卷 25-31页

作者： Xinyi Hu Riguang Zhang Zhao Jiang Department of Chemical Engineering Shaanxi Key Laboratory of Energy Chemical Process IntensificationEngineering Research Center of New Energy System Engineering and Equipment Xi'an Jiaotong UniversityXi'an710049China State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan030000China

Direct methanol fuel cells have the advantages of simple system,convenient operation,high conversion rate and low carbon emission,which are considered as the environmental and friendly energy conversion ***-ever,the low activity,CO-tolerance and high cost of anode catalysts restrict the large-scale commercial ***,it is of great practical significance to design and construct the anodic catalysts with high activity,stability and low cost for methanol oxidation *** this work,the PtM/Nb_(2)O_(5)-C(M=Co,Sn,Ni)catalysts are synthesized by the ethylene glycol solvothermal method using transition metal oxide Nb_(2)O_(5)as the *** catalytic performance of different catalysts is further evaluated for alkaline *** results show that the introduction of Ni(existing in Ni^(2+)and Ni^(3+))has the most obvious improvement for alkaline MOR *** adjusting the doped ratio of Pt:Ni,it is shown that PtNi/Nb_(2)O_(5)-C has the highest mass activity(3877.9 mA-mg_(pt)^(-1)),12 times that of the commercial Pt/C ***,LSV,Tafel and EIS analyses show that PtNi/Nb_(2)O_(5)-C has the lowest onset potential and charge transfer resistance,and the fastest electrocatalytic oxidation rate of *** tests show that the electrochemical stability is also significantly improved with the introduction of Nb_(2)O_(5)and *** with the structural characterization and electrochemical tests,it is found that the evident electronic effect among Pt and Ni,Nb_(2)O_(5)and the hydroxyl brought from Ni species are mainly ascribed for enhancing the activity,CO resistance and stability of PtNi/Nb_(2)O_(5)-C.

关键词： Direct methanol fuel cell Niobium oxide Platinum-based catalysts Methanol oxidation reaction

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GPU-enhanced DEM analysis of flow behaviour of irregularly shaped particles in a full-scale twin screw granulator

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Particuology 2022年第2期20卷 30-40页

作者： Chao Zheng Nicolin Govender Ling Zhang Chuan-Yu Wu Department of Chemical and Process Engineering University of SurreyGuildford GU27XHUnited Kingdom Department of Mechanical Engineering University of JohannesburgSouth Africa Research Center Pharmaceutical Engineering GmbH Graz 8010Austria

During twin screw granulation(TSG),small particles,which generally have irregular shapes,agglomerate together to form larger granules with improved ***,how particle shape impacts the conveying characteristics during TSG is not explored nor well *** this study,a graphic processor units(GPUs)enhanced discrete element method(DEM)is adopted to examine the effect of particle shape on the conveying characteristics in a full scale twin screw granulator for the first *** is found that TSG with spherical particles has the smallest particle retention number,mean residence time,and power consumption;while for TSG with hexagonal prism(Hexp)shaped particles the largest particle retention number is obtained,and TSG with cubic particles requires the highest power ***,spherical particles exhibit a flow pattern closer to an ideal plug flow,while cubic particles present a flow pattern approaching a perfect *** is demonstrated that the GPU-enhanced DEM is capable of simulating the complex TSG process in a full-scale twin screw granulator with non-spherical particles.

关键词： Discrete element method Twin screw granulation Non-spherical particle Residence time distribution GPU

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Two-dimensional RGO-bridge S-scheme phosphorus-doped g-C_(3)N_(4)/Bi_(5)O_(7)Ivan der Waals heterojunctions for efficient visible-light photocatalytic treatment of real pharmaceutical wastewater

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Science China(Technological Sciences) 2023年第10期66卷 3011-3024页

作者： WANG ZhenZhou XU XiWei DENG Fang DIONYSIOU Dionysios D LI XiBao PENG JunLong LUO XuBiao ZOU JianPing LUO ShengLian National-Local Joint Engineering Research Center of Heavy Metal Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China Environmental Engineering and Science Program Department of Chemical and Environmental Engineering(DChEE)University of CincinnatiCincinnati 45221-0012USA

The design of van der Waals heterojunctions with S-scheme charge transfer pathway is expected to be an effective strategy for improvement of photocatalytic ***,two-dimensional(2D)phosphorus-doped g-C_(3)N_(4)/Bi_(5)O_(7)Ivan der Waals heterojunctions with reduced graphene oxide as electron bridge(PCN/RGO/Bi_(5O)_(7)I)were successfully synthesized via hydrothermal *** van der Waals interaction endowed 2D PCN/RGO/Bi_(5O)_(7)I with intimate contact interface,lattice match,tunable band structure,and internal electric field,which efficiently promoted interfacial charge separation and enhanced redox ability of photogenerated charge *** a result,the S-scheme PCN/RGO/Bi_5O_7I van der Waals heterojunctions exhibited superior photocatalytic performance in ciprofloxacin degradation and real pharmaceutical wastewater *** optimized 12%PCN/RGO/Bi_5O_7I displayed the highest photocatalytic activity with 92%removal of ***,the COD removal efficiency and extent of mineralization of real pharmaceutical wastewater reached 66.9%and 59.8%,respectively,and the biodegradability of pharmaceutical wastewater was significantly *** photocatalytic mechanism of the S-scheme PCN/RGO/Bi_(5)O_(7)I van der Waals heterojunctions based on the analysis of reactive species,work function,and internal electric field was *** study provides fresh insights into plausible design of S-scheme van der Waals heterojunction to enhance photocatalytic redox ability.

关键词： S-scheme heterojunction van der Waals heterostructure photocatalytic degradation ciprofloxacin energy consumption

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