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Catalytic co-combustion of biomass and brown coal in a fluidized bed:Economic and environmental benefits

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Journal of Environmental Sciences 2024年第6期140卷 24-36页

作者： Yury V.Dubinin Nikolay A.Yazykov Petr M.Yeletsky Roman B.Tabakaev Aleksandra I.Belyanovskaya Vadim A.Yakovlev Federal research center Boreskov Institute of catalysis SB RAS Lavrentiev Ave.5Novosibirsk630090Russia University of Tyumen Volodarskogo str.6Tyumen625003Russia

The work is devoted to the study of combustion of brown coal,pine sawdust,and their mixtures in a fluidized bed of catalyst at 600-750℃.It is shown that an increase in the content of sawdust in a mixture with brown coal leads to an increase in the burnout degree of solid fuel from 94.4%to 99.9%,while the emission of greenhouse gases in the form of CO_(2)CO and NOxis reduced(CO_(2)from the biomass is not included in the balance).The high content of alkaline earth metal oxides(CaO and MgO)in the mineral part of brown coal,sawdust,and their mixtures eliminates the emission of sulfur oxides and the slagging of heat-exchange surfaces during the combustion in a fluidized bed of catalyst.The optimal temperature,when the highest burnout degree of the above fuels is achieved in the combustion is 750℃.It is also shown that the increase in temperature and the content of sawdust in the composition of the fuel mixtures has a positive effect on the economic and environmental process indicators.

关键词： Co-combustion Fluidized catalyst bed Biomass Coal Economic effect Environmental impact

Tuning interaction strength between CeO_(2) and iridium to promote CO oxidation over Ir/TiO_(2)

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Journal of Rare Earths 2024年第4期42卷 651-659页

作者： Lu Dai Binghua Li Yuhan Peng Xianwei Hao Runquan Xuan Hua Huang Yiming Bi Liping Xu Yanhui Zhang Yun Guo Fangqi Du Li Wang Hui Wang Technology center China Tobacco Zhejiang Industrial Co.Ltd.Hangzhou310024China research Institute of Industrial catalysis East China University of Science and TechnologyShanghai200237China

The interaction between support and noble metal plays a crucial role in heterogeneous catalysis design.However,how to tune metal support interactions to optimize the activity still needs further exploration.CeO_(2) was introduced to promote CO oxidation ove r Ir/TiO_(2) by adjusting the interaction strength between iridium(Ir)and CeO_(2).The strong interaction between Ir and CeO_(2) blocks CO adsorption and causes low CO oxidation activity.However,introducing CeO_(2) on Ir/TiO_(2) produces localized interaction between Ir and CeO_(2),which can tune the surface electronic state of Ir,so a"volcano curve"relationship between CO oxidation activity and electronic state is built.Limited amount of CeO_(2) on Ir/TiO_(2)(Ir/Ce_(0.2)Ti)leads to CO complete oxidization at 22℃,and a new pathway for CO oxidation was explored.The study demonstrates that the utilization of tuning interaction strength between active metal and support is a potential method to increase the catalytic activity.

关键词： CO oxidation CeO_(2) Localized interaction Interaction strength Supported Ir catalysts Rareearths

A critical review towards the causes of the iron-based catalysts deactivation mechanisms in the selective oxidation of hydrogen sulfide to elemental sulfur from biogas

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Journal of Energy Chemistry 2024年第3期90卷 388-411,I0010页

作者： Mostafa Tarek Janaina S.Santos Victor Márquez Mohammad Fereidooni Mohammad Yazdanpanah Supareak Praserthdam Piyasan Praserthdam center of Excellence on catalysis and Catalytic Reaction Engineering(CECC) Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailan High-Performance Computing Unit(CECC-HCU) Center of Excellence on Catalysis and Catalytic Reaction Engineering(CECC)Chulalongkorn UniversityBangkok 10330Thailand

Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low concentrations.Among various technologies,the selective oxidation of hydrogen sulfide(SOH_(2)S) to elemental sulfur(S) has emerged as a sustainable and environmentally friendly solution.Due to its unique properties,iron oxide has been extensively investigated as a catalyst for SOH_(2)S;however,rapid deactivation has remained a significant drawback.The causes of iron oxide-based catalysts deactivation mechanisms in SOH_(2)S,including sulfur or sulfate deposition,the transformation of iron species,sintering and excessive oxygen vacancy formation,and active site loss,are thoroughly examined in this review.By focusing on the deactivation mechanisms,this review aims to provide valuable insights into enhancing the stability and efficiency of iron-based catalysts for SOH_(2)S.

关键词： Selective oxidation of H_(2)S Iron-based Catalysts Mechanism of deactivation Sulfur or sulfate deposition Transformation of iron species Sintering SDG 7

Feasibility of low-intensity ultrasound treatment with hydroxylamine to accelerate the initiation of partial nitrification and allow operation under intermittent aeration

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Journal of Environmental Sciences 2024年第5期139卷 446-459页

作者： Jianxiong Jian Xiaojian Liao Zhihua Mo Shoupeng Li Lei Li Shaojin Chen Zhenhua Huang Junhao Chen Wencan Dai Shuiyu Sun Guangzhou Key Laboratory Environmental catalysis and Pollution Control Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlSchool of Environmental Science and EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangdong Province Solid Waste Recycling and Heavy Metal Pollution Control Engineering Technology research center Guangdong Polytechnic of Environmental Protection EngineeringFoshan 528216China Analysis and Test center Guangdong University of TechnologyGuangzhou 510006China

Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial nitrification.Results showthat compared with the control group,low-intensity ultrasound treatment(0.10W/mL,15 min)combined with NH2OH(5 mg/L)reduced the time required for partial nitrification initiation by 6 days,increasing the nitrite accumulation rate(NAR)and ammonia nitro-gen removal rate(NRR)by 20.4% and 6.7%,respectively,achieving 96.48% NRR.Mechanis-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification initiation.Furthermore,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass transfer.In addition,16S rRNA gene sequencing results showed that ultrasonication-sensitive Nitrospira disappeared from the ultrasound+NH_(2)OH system,while Nitrosomonas gradually became the dominant group.Collectively,the results of this study provide valuable insight into the enhancement of partial nitrification start-up during the process of wastewater nitrogen removal.

关键词： Partial nitrification Low-intensity ultrasound Hydroxylamine Ammonia oxidizing bacteria Nitrite oxidizing bacteria

Developing silicon-based photocathodes for CO_(2) conversion

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Science China Chemistry 2024年第6期67卷 1904-1921页

作者： Weijie Zhuang Miao Kan Tao Meng Jinlong Zhang Key Laboratory for Advanced Materials and Joint International research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China Shanghai Engineering research center for Multimedia Environmental catalysis and Resource Utilization East China University of Science and TechnologyShanghai200237China

Photoelectrochemical(PEC)conversion of CO_(2) presents a promising avenue for solar-driven chemical fuel production,with silicon emerging as a cost-effective and high-light-absorbing material pivotal to this technology.Aiming at exploring opportunities for industrializing PEC CO_(2) reduction(PEC-CO_(2)R)by minimizing reaction energy consumption,enhancing reaction efficiency and selectivity,this review summarizes recent advancements in developing Si-based photocathodes for PEC-CO_(2)R.It outlines the fundamental principles,advantages,and limitations of Si photocathodes with key performance metrics.Based on this understanding,the strategies to enhance the performance of the PEC-CO_(2)R system,including light absorption,charge separation,and catalytic reactions are categorized as the interfacial modification,active site decoration,and protective layer design.The design ideas of this advantageous three-layer structure in promoting the efficiency,stability,and selectivity have been clarified.Then,this review scrutinizes the influence of the photocathodic chemical environment.This review consolidates the mechanism insights and notable breakthroughs of various fuel generation processes within Si-based PEC-CO_(2)R systems.Providing this wealth of information offers an up-to-date perspective on the dynamic developments in silicon-based PEC-CO_(2) conversion and underscores the promising pathways toward the sustainable fuel synthesis from pollutant CO_(2).

关键词： photoelectrochemistry solar fuels silicon photocathodes carbon dioxide reduction microenvironment

Photodegradation of xylene isomers:Kinetics,mechanism,secondary pollutant formation potential and health risk evaluation

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Journal of Environmental Sciences 2024年第2期136卷 658-669页

作者： Xiaoyan Chen Weikun Zhu Sufen Feng Jiangyao Chen Guangdong Key Laboratory of Environmental catalysis and Health Risk Control Guangdong Technology Research Center for Photocatalytic Technology Integration and Equipment EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of Environmental catalysis and Pollution Control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.

关键词： Isomer aromatics Photodegradation Ozone formation Secondary organic aerosols Health risk

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 protons.Diverging 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 silanes.As the synthesis of diverse catalytic progress,the categories of donors have seen rapid expansion.However,existing literature only provides summaries regarding the metal,ligands,and mechanism.Despite the significance of electron and proton donor combinations in nitrogen reduction reactions,no literature has thoroughly reviewed this aspect.Therefore,we hereby compiled a comprehensive list of commonly used reagents in N_(2)reduction and classified them according to their specific donor combinations.This review presents clear and organized information about these combinations,along with a summary of their general performance trend in NRR with related catalysts.Finally,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

Investigation of Ce/BEA as a passive NOx adsorber:1.The occurrences of cerium and adsorption behavior

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Journal of Rare Earths 2024年第7期42卷 1265-1271页

作者： Minghui Yu Yiying Ding Xiaojie Yu Siwei Yan Meiqing Shen Jianqiang Wang Jun Wang Gurong Shen School of Materials Science and Engineering Tianjin University School of Chemical Engineering and Technology Tianjin University National Rare Earth catalysis research Institute

Ce/BEA has great potential as a passive NOxabsorber（PNA） to reduce the NOxemissions during the cold start phase especially in diesel engine for its high resistance to CO and suitable NOxdesorption temperature range.However,as a novel material,its physical and chemical properties still remain unknown.In this work,Ce/BEA was synthesized by ion-exchange method to identify the active species in NOxadsorption,compared with aggregated Ce species in Ce/SiAlOxprepared by impregnation method.X-ray diffraction（XRD）,high resolution-transmission electron microscopy（HR-TEM） and aberration-correctedscanning transmission electron microscopy（AC-STEM） were performed to confirm the isolated single atom formation of Ce species in Ce/BEA.UV-vis diffraction reflection spectra（DRS） and X-ray photoelectron spectroscopy（XPS） were conducted to find the difference of chemical environment between the isolated Ce species and aggregated ones.PNA performance evaluation and temperature programmed reduction of hydrogen（H2-TPR） results show the high NOxstorage capacity and active oxygen species quantity in Ce/BEA.It is also found that the main NOxadsorption species are Ce4+-O*rather than Ce3+.NOx-diffuse reflectance infrared Fourier transform spectroscopy（NOx-DRIFTS） confirms that the bidentate nitrite species are the critical NOxadsorption intermediates and the conception of NOxadsorption and desorption processes is proposed.

关键词： Ce/BEA Isolated Ce species Passive NOx absorber Rare earths

Engineering the Interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic Performance of 5-Hydroxymethylfurfural(HMF)to 2,5-Dimethylfuran(DMF)

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Chemical research in Chinese Universities 2024年第1期40卷 47-54页

作者： XIANG Shuang GUO Yong LIU Xiaohui WANG Yanqin Key Laboratory for Advanced Materials and Joint International research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis reactions.Herein,we create the Au-CoO-OV interface in the 1.0%Au/Co3O4-Rod-250 catalyst,which could dissociate H2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2,5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3O4-Rod-250).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)