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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

In-situ fabrication of TiO2/NH2-MIL-125（Ti） via MOF-driven strategy to promote efficient interfacial effects for enhancing photocatalytic NO removal activity

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Chinese Chemical Letters 2024年第10期35卷 415-419页

作者： Maosen Xu Pengfei Zhu Qinghong Cai Meichun Bu Chenghua Zhang Hong Wu Youzhou He Min Fu Siqi Li Xingyan Liu Chongqing Key Laboratory of catalysis and New environmental materials College of Environment and Resources Chongqing Technology and Business University School of Pharmacy North Sichuan Medical College State Key Joint Laboratory of environment Simulation and Pollution Control School of Environment Tsinghua University

Deep oxidation of NO molecules to nitrate species by photocatalysis with virtually no toxic byproduct NO2generation is a challenging task. In this study, Ti O2in-situ grows based on NH2-MIL-125（Ti）(NM-125) not only inhibited TiO 2agglomeration, but also contacted more tightly to obtain efficient interfacial effects, thus displaying excellent photocatalytic NO removal activity（68.08%）. The formation of Ti O2is directly confirmed by characterizations such as X-ray diffraction（XRD）, transmission electron microscope（TEM）, X-ray photoelectron spectroscopy（XPS）. Meanwhile, UV–vis, photoluminescence, and photoelectrochemical analysis indicate that TiO2formation effectively improves the optical properties. Moreover,the strong electron interaction and electron transport direction between NM-125 and Ti O2are investigated by density functional theoretical（DFT） calculation. Finally, combined with the results of electron spin resonance（ESR） and in-situ FT-IR test, the intermediate processes of NO adsorption and photocatalytic oxidation reaction are discussed in depth, where the production of reactive oxygen species（ROS）under light is the key factor in the successful degradation of NO. Compared with NM-125 which can only produce·OH through photogenerated electrons since the lower valence band position, NMT-2 can directly produce·OH through photogenerated holes, thereby relieving the pressure on photogenerated electrons and producing more ROS. This study will provide reasonable guidance for the modification of NM-125 for photocatalytic removal of ppb-level NO.

关键词： NH2-MIL-125(Ti) NO removal Photocatalysis ROS TiO2

A review of low-carbon technologies and projects for the global cement industry

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Journal of environmental Sciences 2024年第2期136卷 682-697页

作者： Yangyang Guo Lei Luo Tingting Liu Liwei Hao Yinming Li Pengfei Liu Tingyu Zhu CAS Key Laboratory of Green process and Engineering Institute of Process EngineeringInnovation Academy for Green ManufactureChinese Academy of SciencesBeijing 100190China Center for Excellence in Regional Atmospheric environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China State Key Laboratory of Solid Waste Reuse for Building materials Beijing Building Materials Academy of Sciences ResearchBeijing 100041China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China

Carbon dioxide(CO_(2))emissions from the cement industry account for 26%of the total industrial emissions,and the need to develop low-carbon techniques within the cement industry is extremely ***-carbon projects and technologies for the cement industry in different regions and countries have been thoroughly reviewed in this manuscript,and the low-carbon development concept for each county has been *** developing countries such as China and India,energy saving and efficiency enhancement are currently the key points,while for developed countries and regions such as Europe,more efforts have been focused on carbon capture,utilization,and storage(CCUS).Global CCUS projects have been previously conducted,and the majority of CCUS projects are currently performed in Europe where major projects such as the CEMCAP,CLEANKER,and IEILAC projects represent the latest research progress in cement production technologies and low-carbon technologies for the global cement *** development of low-carbon cement technologies has changed from focusing on the end point to instead focusing on the source and process through the exploration of hydrogen and solar energies,and more disruptive and original technologies are expected to be developed,particularly in the cement industry in China.

关键词： Cement industry CO_(2)emissions Low carbon development Projects Carbon capture utilization and storage

Pd Pt VO_(x)/CeO_(2)-ZrO_(2):Highly efficient catalysts with good sulfur dioxide-poisoning reversibility for the oxidative removal of ethylbenzene

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Journal of environmental Sciences 2024年第4期138卷 153-166页

作者： Jia Wang Yuxi Liu Jiguang Deng Lin Jing Xiuqing Hao Xing Zhang Xiaohui Yu Hongxing Dai Beijing Key Laboratory for Green catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various *** activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,*** large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/*** activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut *** good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.

关键词： Ceria-zirconia Supported palladium-platinum-vanadium catalyst Volatile organic compound Ethylbenzene oxidation Sulfur dioxide resistance

Insight into Lithium–sulfur batteries performance enhancement: from metal nanoparticles to metal nanoclusters to single metal atoms

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Tungsten 2024年第3期6卷 504-521页

作者： Shuang Ma Qing-Ling ruan Xue-Cheng Liu Gui-Jun Zhu Die Yuan Ling-Qiao Hu Yu-Mei Huang Xing-Xing Gu Chongqing Key Laboratory of catalysis and New environmental materials College of Environment and Resources Chongqing Technology and Business University National Research Base of Intelligent Manufacturing Service Chongqing Technology and Business University

Lithium-sulfur(Li-S) batteries have attracted much attention and developed rapidly in recent years due to their high energy density,low cost,and ***,its commercialization process still encounters various *** them,the sulfur cathode is easy to dissolve and shuttle,resulting in the loss of active substances and the severe growth of lithium anode dendrites,which is one of the biggest *** the redox conversion kinetics of sulfur cathode is expected to fundamentally alleviate the shuttle phenomenon of poly ***,this paper reviews the effects of metal nanoparticles to metal nanoclusters to metal single-atom catalysts on improving the redox of Li-S batteries,to let researchers better understand the size effect on the kinetics of sulfur cathodes in Li-S batteries,which will provide important guidance for the future large-scale commercialization of Li-S batteries.

关键词： Lithium–sulfur batteries Metal nanoparticles Metal nanoclusters Metal single atoms Size effects

From ore to MOF: A case of MIL-100(Fe) production from iron ore concentrates

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Progress in Natural Science:materials International 2024年第01期34卷 66-73页

作者： Miao Chang Chiyao Tang Chong-Chen Wang Chen Zhao Beijing Key Laboratory of Functional materials for Building Structure and environment Remediation School of Environment and Energy Engineering Beijing University of Civil Engineering and Architecture

Within this work, iron ore concentrates instead of elemental iron Fe0and iron salts like Fe（NO3）3and FeCl3were selected as iron source to prepare MIL-100（Fe）(labeled as MIL-100（Fe）-ore). The corresponding synthesis cost is reduced to half of the MIL-100（Fe） produced from elemental iron and iron salts. As well, the unreacted iron ore concentrates can be easily separated from the as-prepared MIL-100（Fe）-ore by magnetic to facilitate the purification process, free of the strong acids to wash the residual iron. The as-obtained MIL-100（Fe）-ore with Langmuir surface area up to 2281.6 m2g-1displayed long-term chemical stability. Furthermore, the sorption capacity of MIL-100（Fe）-ore towards malachite green（MG） is up to 522.3 mg g-1at 25℃ and initial pH = 3.2, higher than that of MIL-100（Fe） yielded by conventional hydrothermal process. Finally, the production cost and life cycle assessment of MIL-100（Fe）-ore were compared with other traditional production procedures. The results revealed that our work greatly reduced the synthesis cost and enhanced the environmental sustainability.

关键词： Metal-organic framework Iron ore concentrates Adsorption Life cycle assessment

Combinations of electron and proton donors in transition-metal complex mediated nitrogen reduction reactions

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Science China Chemistry 2024年第7期67卷 2136-2154页

作者： Delong Han Li Yang Hao Huang Priyanka Chakraborty Shashikant U.Dighe Kuo-Wei Huang KAUST catalysis Center and Division of Physical Science and Engineering King Abdullah University of Science and TechnologyThuwal 23955Saudi Arabia Agency for Science Technologyand ResearchInstitute of Materials Research and Engineering and Institute of Sustainability for ChemicalsEnergy and EnvironmentSingapore 138634Singapore

Nitrogen fixation is a complex process involving the transfer of six electrons and *** from the conventional Haber-Bosch process,which relies on hydrogen(H_(2))to provide both electrons and protons to reduce nitrogen(N_(2)),homogeneous transition metal complex-catalyzed N_(2)reduction reactions(NRR)employ an array of electron and proton donors or even electron donors combined with *** the synthesis of diverse catalytic progress,the categories of donors have seen rapid ***,existing literature only provides summaries regarding the metal,ligands,and *** the significance of electron and proton donor combinations in nitrogen reduction reactions,no literature has thoroughly reviewed this ***,we hereby compiled a comprehensive list of commonly used reagents in N_(2)reduction and classified them according to their specific donor *** review presents clear and organized information about these combinations,along with a summary of their general performance trend in NRR with related ***,we conclude the discussion by highlighting key points for researchers to consider when selecting catalysts and donor combinations,with the ultimate goal of advancing the field of nitrogen fixation.

关键词： dinitrogen reduction reaction reducing donor combination transition metal complexes homogeneous catalysis

Plasma-assisted ammonia synthesis under mild conditions for hydrogen and electricity storage:Mechanisms,pathways,and application prospects

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Frontiers in Energy 2024年第4期18卷 418-435页

作者： Feng GONG Yuhang JING rui XIAO Key Laboratory of Energy Thermal Conversion and process Measurement and Control of the Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing 210096China

Ammonia,with its high hydrogen storage density of 17.7 wt.%(mass fraction),cleanliness,efficiency,and renewability,presents itself as a promising zero-carbon ***,the traditional Haber−Bosch(H−B)process for ammonia synthesis necessitates high temperature and pressure,resulting in over 420 million tons of carbon dioxide emissions annually,and relies on fossil fuel *** contrast,dielectric barrier discharge(DBD)plasma-assisted ammonia synthesis operates at low temperatures and atmospheric pressures,utilizing nitrogen and hydrogen radicals excited by energetic electrons,offering a potential alternative to the H−B *** method can be effectively coupled with renewable energy sources(such as solar and wind)for environmentally friendly,distributed,and efficient ammonia *** review delves into a comprehensive analysis of the low-temperature DBD plasma-assisted ammonia synthesis technology at atmospheric pressure,covering the reaction pathway,mechanism,and catalyst system involved in plasma nitrogen *** from current research,it evaluates the economic feasibility of the DBD plasmaassisted ammonia synthesis technology,analyzes existing dilemmas and challenges,and provides insights and recommendations for the future of nonthermal plasma ammonia processes.

关键词： plasma catalysis nitrogen fixation ammonia synthesis hydrogen storage catalyst carbon neutralization

Enlarged interlayer of separator coating enabling high-performance lithiumsulfur batteries

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Frontiers of Chemical Science and Engineering 2024年第2期18卷 103-112页

作者： Yanqi Feng Hui Liu Xiaoting Liu Qiongqiong Lu School of materials&environment Engineering Chengdu Technological UniversityChengdu 611730China School of materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Green catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Institute of materials Henan Key Laboratory of Advanced Conductor MaterialsHenan Academy of SciencesZhengzhou 450046China Leibniz Institute for Solid State and materials Research(IFW) Dresden e.V.Dresden 01069Germany

Lithiumsulfur batteries have been intensively studied due to their high theoretical energy density and abundant sulfur resources. However, their commercial application is hindered by the low redox kinetics and high sulfur losses. In principle, in the design of cathodes and separators, the adsorption toward lithium-polysulfides should be enhanced and the conversion of soluble high-order lithium-polysulfides should be catalyzed. Herein, a KV_(3)O_(8)·0.75H_(2)O separator is designed as an effective lithium-polysulfides mediator in lithiumsulfur batteries. The intercalated K+ would enlarge the interlayer spacing of vanadium oxides, preventing the collapse of the layer structure and improving the electrical/ion conductivity of the interface. Moreover, the KV_(3)O_(8)·0.75H_(2)O modified separator possess a prior adsorption and high redox kinetics toward lithium-polysulfides due to the enhanced diffusion kinetics, which guarantees the high-rate capability and efficient utilization of sulfur. As a result, lithiumsulfur batteries exhibit a high capacity of 1362 mAh·g^(-1) and a long lifespan with a low capacity loss of 0.073% per cycle. This work may provide an alternative way to establish a functional separator to balance the adsorption and conversion of polysulfides during the redox back and forth.

关键词： lithium kinetics adsorption