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In-situ synthesis of N, S co-doped hollow carbon microspheres for efficient catalytic oxidation of organic contaminants

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Chinese Chemical Letters 2022年第3期33卷 1298-1302页

作者： Yongbing Xie Ya Liu Yujie Yao Yanchun Shi Binran Zhao Yuxian Wang State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization Panzhihua 617000China CAS Key Laboratory of Green Process&Engineering Beijing Engineering Research Center of Process Pollution ControlInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China State Key Laboratory of Heavy Oil Processing State Key Laboratory of Petroleum Pollution ControlChina University of Petroleum-BeijingBeijing 102249China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia School of Chemical Engineering Northwest UniversityXi'an 710069China

Metal-free heteroatom doped nanocarbons are promising alternatives to the metal-based materials in catalytic ozonation for destruction of aqueous organic contaminants. In this study, N, S co-doped hollow carbon microspheres (NSCs) were synthesized from the polymerization products during persulfate wet air oxidation of benzothiazole. The contents of doped N and S as well as the structural stability were maneuvered by adjusting the subsequent N_(2)-annealing temperature. Compared with the prevailing single-walled carbon nanotubes, the N_(2)-annealed NSCs demonstrated a higher catalytic ozonation activity for benzimidazole degradation. According to the quantitative structure-activity relationship (QSAR) analysis, the synergistic effect between the graphitic N and the thiophene-S which redistributed the charge distribution of the carbon basal plane contributed to the activity enhancement of the N_(2)-annealed NSCs. Additionally, the hollow structure within the microspheres served as the microreactor to boost the mass transfer and reaction kinetics via the nanoconfinement effects. Quenching and electron paramagnetic resonance (EPR) tests revealed that benzimidazole degradation was dominated by the produced singlet oxygen (^(1)O_(2)) species, while hydroxyl radicals (^(·)OH) were also generated and participated. This study puts forward a novel strategy for synthesis of heteroatom-doped nanocarbons and sheds a light on the relationship between the active sites on the doped nanocarbons and the catalytic performance.

关键词： Metal-free catalysis Hollow carbon microspheres N,S co-doping Catalytic ozonation Singlet oxygen(1O_(2))

Ni nanoparticles encapsulated within H-type ZSM-5 crystals for upgrading palmitic acid to diesel-like fuels

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Chinese Chemical Letters 2022年第2期33卷 803-806页

作者： Yanchun Shi Chen Gao Enhui Xing Jimei Zhang Feng Duan He Zhao Yongbing Xie CAS Key Laboratory of Green Process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China State Key Laboratory of Catalytic Materials and Reaction Engineering Research Institute of Petroleum ProcessingSinopecBeijing 100083China

Meso-Ni@HZSM-5 bi-functional catalysts were successfully post-encapsulated with about 3-7 nm Ni nanoparticles within HZSM-5 crystals,which exhibited significantly efficient conversion activity(67.4 g[palmitic acid]g[Ni]^(−1)h^(−1))of palmitic acid and 100%selectivity of hydrocarbons with the outstanding stability during recycling application,compared to the impregnated Ni/HZSM-5 catalyst(14.0 g[palmitic acid]g[Ni]^(−1)h^(−1)).

关键词： Post-encapsulation Ni@HZSM-5 Ni nanoparticles Palmitic acid Hydrodeoxygenation Hydrocarbons

A facial synthesis of nitrogen-doped reduced graphene oxide quantum dot and its application in aqueous organics degradation

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Green Energy & Environment 2022年第3期7卷 440-448页

作者： He Zhao Juehua Wang Zhuangjun Fan Yongbing Xie Di Zhang Shanshan Sun Yi Zhang Hongbin Cao CAS Key Laboratory of Green Process and Engineering Institute of Process EngineeringInnovation Academy for Green ManufactureChinese Academy of SciencesBeijing Engineering Research Centre of Process Pollution ControlBeijing100190China University of Chinese Academy of Sciences Beijing100049China School of Materials Science and Engineering China University of Petroleum(East China)QingdaoShandong266580China

N-doped reduced graphene oxide quantum dots(N-rGQDs) have attracted more and more attention in efficient catalytic degradation of aqueous organic pollutants.However,the synthesis of N-rGQDs is generally a complex and high energy required process for the reduction and N-doping steps.In this study,a facile and green fabrication approach of N-rGQDs is established,based on a metal-free Fenton reaction without additional energy-input.The N structures of N-rGQDs play a significant role in the promotion of their catalytic performance.The N-rGQDs with relatively high percentage of aromatic nitrogen(NAr-rGQDs) perform excellent catalytic activities,with which the degradation efficiency of pollutant is enhanced by 25 times.Density functional theory(DFT) calculation also indicates aromatic nitrogen structures with electron-rich sites are prone to transfer electron,presenting a key role in the catalytic reaction.This metal-free Fenton process provides a green and costeffective strategy for one-step fabrication of N-rGQDs with controllable features and potential environmental catalytic applications.

关键词： reaction quantum synthesis

Reaction mechanism and metal ion transformation in photocatalytic ozonation of phenol and oxalic acid with Ag^+/TiO_2

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Journal of Environmental Sciences 2014年第3期26卷 662-672页

作者： Yingying Chen Yongbing Xie Jun Yang Hongbin Cao Yi Zhang National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences University of Chinese Academy of Sciences State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences

Photocatalytic ozonation of phenol and oxalic acid （OA） was conducted with a Ag^＋/TiO2 catalyst and different pathways were found for the degradation of different compounds. Ag^＋ greatly promoted the photocatalytic degradation of contaminants due to its role as an electron scavenger. It also accelerated the removal rate of OA in ozonation and the simultaneous process for its complex reaction with oxalate. Phenol could be degraded both in direct ozonation and photolysis, but the TOC removal rates were much higher in the simultaneous processes due to the oxidation of hydroxyl radicals resulting from synergetic effects. The sequence of photo-illumination and ozone exposure in the combined process showed quite different effects in phenol degradation and TOC removal. The synergetic effects in different combined processes were found to be highly related to the properties of the target pollutants. The color change of the solution and TEM result confirmed that Ag＋ was easily reduced and deposited on the surface of Tit2 under photo-illumination, and dissolved again into solution in the presence of ozone. This simple cycle of enrichment and distribution of Ag^＋ can greatly benefit the design of advanced oxidation processes, in which the sequences of ozone and photo-illumination can be varied according to the needs for catalyst recycling and the different properties of pollutants.

关键词： photocatalytic ozonation phenoloxalic acid Ag＋/TiO2

Insights into the floatability between spodumene and albite from crystal chemistry standpoint

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International Journal of Mining Science and Technology 2022年第6期32卷 1329-1339页

作者： Hepeng Zhou Fanxin xie yongbing Zhang Boyuan Zhang Siqi Yang Xianping Luo Engineering Research Center for High-efficiency Development and Application Technology of Tungsten Resources(Jiangxi University of Science and Technology) Ministry of EducationGanzhou 341000China Jiangxi Province Key Laboratory of Mining and Metallurgy Environmental Pollution Control Jiangxi University of Science and TechnologyGanzhou 341000China

Spodumene is a silicate mineral rich in lithium.However,the gangue mineral,albite has similar crystal chemical structure and composition to spodumene.In this work,the density functional theory(DFT)calculation was taken to research the floatability from the perspective of crystal chemistry.And contact angle test and reagent adsorption test were used to support the simulation results.In addition,the weighted total density of broken bonds is proposed for the first time to judge the generation probability of cleavage surface.The DFT calculation results display that the Na and Al sites on the albite surface are the adsorption sites of water molecules.While the water molecules only bond with Al atom on the surface of spodumene and each Al site can adsorb only one water molecule.Thus,the wetting effect of water molecules on the albite surface is stronger than that of spodumene.This is consistent with the result of contact angle.In sodium oleate system,the oleic acid anion is adsorbed on the spodumene surface in form of a multicomponent ring while the albite is a single ring.Theoretically,oleic acid anion can be strongly adsorbed on the surface of spodumene and albite under vacuum.The adsorption strength of spodumene is higher than that of albite.However,on hydrated surface,the adsorption strength of oleic acid anion on mineral surface is greatly reduced due to the interaction between water molecules and metal site on mineral surface.Thus,spodumene and albite are hard to float without external activated ions in sodium oleate system.

关键词： Spodumene Albite Floatability Crystal chemistry DFT calculation

Dendritic BiVO4 decorated with MnOx co-catalyst as an efficient hierarchical catalyst for photocatalytic ozonation

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Frontiers of Chemical Science and Engineering 2019年第1期13卷 185-191页

作者： Jin Yang Xuelian Liu Hongbin Cao Yanchun Shi Yongbing Xie Jiadong Xiao School of Chemical Engineering and Technology Tianjin University Tianjin 300072 China Beijing Engineering Research Center of Process Pollution Control CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China

An appropriate co-catalyst can significantly promote the photocatalytic efficacy, but this has been seldom studied in the visible-light photocatalysis combined with ozone, namely photocatalytic ozonation. In this work, a dendritic bismuth vanadium tetraoxide (BiVO4) material composited with highly dispersed MnOv nanoparticles was synthesized, and its catalytic activity is 86.6% higher than bare BiVO4 in a visible light and ozone combined process. Catalytic ozonation experiments, ultraviolet- visible (UV-Vis) diffuse reflectance spectra and photoluminescence spectra jointly indicate that MnOA plays a triple role in this process. MnOv strengthens the light adsorption and promotes the charge separation on the composite material, and it also shows good activity in catalytic ozonation. The key reactive species in this process is OH, and various pathways for its generation in this process is proposed. This work provides a new direction of catalyst preparation and pushes forward the application of photocatalytic ozonation in water treatment.

关键词： manganese oxide bismuth vanadium tetraoxide photocatalytic ozonation hydroxyl radical cocatalyst

Distinct synergetic effects in the ozone enhanced photocatalytic degradation of phenol and oxalic acid with Fe^(3+)/TiO_2 catalyst

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Chinese Journal of Chemical Engineering 2018年第7期26卷 1528-1535页

作者： Yongbing Xie Yingying Chen Jin Yang Chenming Liu He Zhao Hongbin Cao Beijing Engineering Research Center of Process Pollution Control Division of Environment Technology and Engineering Institute of Process Engineering Chinese Academy of Sciences

In this work, phenol and oxalic acid(OA) degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe^(3+)/TiO_2 catalyst. The ferrioxalate complex formed between Fe^(3+) and oxalate accelerated the removal of OA in the ozonation, photolysis and photocatalytic ozonation process, for its high reactivity with ozone and UV. Phenol was degraded in ozonation and photolysis with limited TOC removal rates, but much higher TOC removal was achieved in photocatalytic ozonation due to the generation of ·OH. The sequence of UV light and ozone in the sequential process also influences the TOC removal, and ozone is very powerful to oxidize intermediates catechol and hydroquinone to maleic acid. Fenton or photo-Fenton reactions only played a small part in Fe^(3+)/TiO_2catalyzed processes, because Fe^(3+) was greatly reduced but not regenerated in many cases.The synergetic effect was found to be highly related with the property of the target pollutants. Fe^(3+)/TiO_2 catalyzed system showed the highest ability to destroy organics, but the TiO_2 catalyzed system showed little higher synergy.

关键词：对苯二酚催化剂臭氧合作草酸 Fenton 分解作用催化系统

Conversion of phenol to cyclohexane in the aqueous phase over Ni/zeolite bi-functional catalysts

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Frontiers of Chemical Science and Engineering 2021年第2期15卷 288-298页

作者： Jimei Zhang Fuping Tian Junwen Chen Yanchun Shi Hongbin Cao Pengge Ning Shanshan Sun Yongbing Xie School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China CAS Key Laboratory of Green Process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China College of Chemistry Dalian University of TechnologyDalian 116024China State Key Laboratory of Catalytic Materials and Reaction Engineering Research Institute of Petroleum ProcessingSINOPECBeijing 100083China

A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation(HDO)of phenol.The Ni dispersibility and particle sizes were shown to be directly related to the porosity and crystal sizes of the parent zeolites,which further influenced the catalytic performances.The large pores and small crystal sizes of the parent zeolites were beneficial for dispersing Ni and forming small Ni particles,and the corresponding Ni/zeolite catalyst exhibited a higher phenol conversion and selectivity towards hydrocarbons.Importantly,the Ni/HIM-5 bi-functional catalyst exhibited a high activity(98.3%)and high selectivity for hydrocarbons(98.8%)when heated at 220°C for 1 h and is thus a new potential catalyst for the HDO of phenolics to form hydrocarbons in the aqueous phase.

关键词： aqueous-phase hydrodeoxygenation phenol hydrocarbons Ni/HIM-5 bi-functional catalyst

Activated carbon enhanced ozonation of oxalate attributed to HO·oxidation in bulk solution and surface oxidation: Effect of activated carbon dosage and pH

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Journal of Environmental Sciences 2014年第10期26卷 2095-2105页

作者： Linlin Xing Yongbing Xie Daisuke Minakata Hongbin Cao Jiadong Xiao Yi Zhang John C. Crittenden National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing Engineering Research Center of Process Pollution Control University of Chinese Academy of Sciences Department of Civil and Environmental Engineering Michigan Technological UniversityHoughton MI 49931 United States School of Civil and Environmental Engineering Brook Byers Institute for Sustainable Systems Georgia Institute of TechnologyAtlantaGA 30332 United States

Ozonation of oxalate in aqueous phase was performed with a commercial activated carbon（AC）in this work. The effect of AC dosage and solution pH on the contribution of hydroxyl radicals（HOU） in bulk solution and oxidation on the AC surface to the removal of oxalate was studied. We found that the removal of oxalate was reduced by tert-butyl alcohol（tBA） with low dosages of AC,while it was hardly affected by tBA when the AC dosage was greater than 0.3 g/L. tBA also inhibited ozone decomposition when the AC dosage was no more than 0.05 g/L, but it did not work when the AC dosage was no less than 0.1 g/L. These observations indicate that HOUin bulk solution and oxidation on the AC surface both contribute to the removal of oxalate. HOU oxidation in bulk solution is significant when the dosage of AC is low, whereas surface oxidation is dominant when the dosage of AC is high. The oxalate removal decreased with increasing pH of the solution with an AC dosage of 0.5 g/L. The degradation of oxalate occurs mainly through surface oxidation in acid and neutral solution, but through HOUoxidation in basic bulk solution. A mechanism involving both HOUoxidation in bulk solution and surface oxidation was proposed for AC enhanced ozonation of oxalate.

关键词： Activated carbon Oxalate Ozonation Hydroxyl radicals Surface oxidation Catalytic ozonation