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Acoustic characterization of hydrate formation and decomposition in clay-bearing sediments

Petroleum Science 2024年第4期21卷 2830-2838页

作者： Yi-Jian Zhu Xiao-Mei Yang Xing Huang Hao Li Xiao-Hui Wang Yi-Fei Sun Peng Xiao Chang-Yu Sun Guang-Jin Chen State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and Environment China University of Petroleum

Understanding the acoustic characteristics of hydrates in various sediments is crucial for hydrate resource detection and safe and efficient exploitation, as hydrate occurrence patterns vary greatly in different sediments. In this work, sediments with different bentonite contents, water saturations, and types were prepared to investigate the characteristics of P-wave velocity(reflecting the magnitude of hydrate saturation in the sediment) and amplitude(reflecting the degree of hydrate-sediment cementation) during hydrate formation and depressurization. During hydrate formation, the P-wave velocity and amplitude have similar trends. As clay content increases, the P-wave velocity increase rates quickened. On the other hand, the increased rate of P-wave velocity slows down with the increase of water saturation in the clay-bearing sediments. Comparing various types of sediment shows that the water absorption and swelling of bentonite reduce the pore space, speeding up the cementation of the hydrate with the sediment and increasing P-wave velocity at a faster rate. Correspondence between P-wave velocity and hydrate saturation is strongly related to sediment type, clay content, and water *** rapidly decreasing amplitude in the early stage of hydrate depressurization indicates that hydrate in clay-bearing sediments is weakly cemented to the sediments, which is prone to stratigraphic *** findings of this study offer guidance for hydrate resource assessments in clay-bearing sediments as well as geologic risk estimations during hydrate mining.

关键词： Gas hydrate Bentonite Illite P-wave velocity Amplitude

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Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao Institute of Catalysis for Energy and environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high *** study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) *** further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and ***,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate *** H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/*** calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational ***,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) *** indicted that the chemisorptions of aldehyde oxygen have largest *** results suggested adsorption conformations have a respectable impact on the catalysis *** study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

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Co-adsorption and selective-adsorption of heavy metals and dyes from aqueous solution by bio-based humus/chitosan hydrogels

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Journal of environmental Sciences 2024年第11期145卷 193-204页

作者： Rongping Chen Chenghao Gan Bingcai Cai Ruxue Liu Wenjie Xu Weize Yin Hongyi Li Lei Yu Qiang Yong college of Biology and the environment Nanjing Forestry UniversityNanjing 210037China college of chemical engineering Nanjing Forestry UniversityNanjing 210037China

An eco-friendly adsorbent was prepared by reverse suspension crosslinking method to remove multiple pollutants from aqueous *** raw materials,derived from humus(HS)and chitosan(CS),are biodegradable and low-cost natural *** combining HS with CS,the adsorption capacity was significantly improved due to compensation effects between the two ***/CS exhibited the features of amphoteric adsorption through pH adjustment,enabling it to adsorb not only anionic pollutants(Methyl Orange(MO)and Cr(VI)),but also cationic ones(Methylene Blue(MB)and Pb(II)).The adsorption capacities were approximately 242 mg/g,69 mg/g,188 mg/g and 57 mg/g for MO,Cr(VI),MB and Pb(II),***/CS showed a slight preference for MO in MO/Cr(VI)co-adsorption system,whereas strong selectivity for MB over Pb(II)in MB/Pb(II)system under acidic condition(pH<3.0).This selective behavior would allow for potential applications in separating MB/Pb(II)effluents and selectively recycling Pb(II)in acidic *** isothermal and kinetic adsorption behaviors followed Langmuir model and pseudo-second-order model,*** density functional theory(DFT)confirmed that the interaction between metal ions and adsorbents was primarily attributed to chelation and electrostatic adsorption,owing to nitric and oxygenic functional ***,the adsorption mechanisms for dyes were involved in electrostatic attraction,H-bond andπ-πbond,due to available hydrogen,oxygen,nitrogen atoms and aromatic groups on the surface of adsorbent and *** adsorbent could be efficiently regenerated and retained over 90%of its adsorption capacity after five cycles,which has a potential for practical applications in water treatment.

关键词： Adsorption Density functional theory(DFT) Humus Chitosan

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Facile fabrication of CdIn_(2)S_(4)/TiO_(2)heterojunction for enhanced solar light efficient CO_(2)reduction

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Frontiers of chemical Science and engineering 2024年第9期18卷 101-112页

作者： Xiaoyu Ma Longlong Wang Houde She Yu Zhou Lei Wang Jingwei Huang Qizhao Wang college of Chemistry and chemical engineering Northwest Normal UniversityLanzhou 730070China School of environment Science and engineering Chang’an UniversityXi’an 710064China

Photocatalytic CO_(2)reduction is a promising solution to simultaneously provide renewable chemical fuels and address the greenhouse ***,designing practical photocatalysts with advanced architectures remains ***,we report the preparation of a novel CdIn_(2)S_(4)/TiO_(2)binary heterojunction via an in situ solvothermal approach,which exhibits superior photocatalytic activity for sunlight-driven CO_(2)*** CdIn_(2)S_(4)/TiO_(2)composites exhibit significantly enhanced photocatalytic performance for CO_(2)reduction compared to unmodified TiO_(2).Among them,the 3%CdIn_(2)S_(4)/TiO_(2)composite has optimal CO and CH_(4) evolution rates of 18.32 and 1.03μmol·g–1·h–1,*** yield of CO is 4.7 times higher than that of pristine TiO_(2).This improved photocatalytic activity of the CdIn_(2)S_(4)/TiO_(2)heterostructure can be attributed to its large surface area,extended light absorption range and high separation efficiency of photogenerated electron-hole pairs,which are supported by the results of photoluminescence spectroscopy and the photoelectrochemical ***,the photocatalytic mechanism based on the binary CdIn_(2)S_(4)/TiO_(2)heterojunction is proposed and separation process of photogenerated electron-hole pairs is *** brief,we aim to provide insights into the application of TiO_(2)in energy conversion processes through the construction of heterogeneous junctions.

关键词： TiiO_(2) CdIn_(2)S_(4) heterojunction photocatalytic CiO_(2)reduction

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Acidic electroreduction CO_(2)to formic acid via interfacial modification of Bi nanoparticles at industrial-level current

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Nano Research 2024年第7期17卷 5817-5825页

作者： Tian Dong Hongdong Li Zhenhui Wang Yanling Geng Rui Chang Xiaofeng Tian Jianping Lai Shouhua Feng Lei Wang Key Laboratory of Eco-chemical engineering International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong engineering Research Center for Marine environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral ***,the proton-rich environment near the catalyst surface favors hydrogen evolution reactions(HER),leading to lower energy efficiency of the desired products,especially in industrial-level current ***,quaternary ammonium cationic surfactant(cetyltrimethylammonium bromide(CTAB))was introduced into acidic electrolyte to modulate the interfacial microenvironment,which greatly enhanced CO_(2)electroreduction to formic acid(HCOOH)at the Bi/C nanoparticles *** a Bi/C nanoparticles electrode with CTAB added,constant production of formic acid was enabled with a cathodic energy efficiency of>40%and maximum FE_(HCOOH)(FE=Faradaic efficiency)of 86.2%at−400 mA·cm^(−2)over 24 *** with in-situ attenuated total reflection Fourier transform infrared spectroscopy,the concentration of*OCHO intermediates significantly increased after CTAB modification,confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO_(2)RR to HCOOH.

关键词： acidic media CO_(2)electrolysis electrolyte additive hydrophobic interfacial microenvironment industrial-level current

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Mixing effects of high-speed jets in gas-solid riser and downer reactors

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Particuology 2024年第9期92卷 196-209页

作者： Zihan Yan Dongdong Wang Lining Wu Chunxi Lu college of chemical engineering and environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China

For the high-temperature and short-contact time gas-solid reaction process,riser and downer are considered appropriate *** realize an intensive and complete mixing of reactants with catalysts,the feed raw is always introduced in the form of high-speed *** this study,in order to investigate the mixing effects of different types of high-speed jets in riser and downer,traceable ozone is injected with the high-speed feed jets to react with catalyst *** detecting the decomposition of ozone,the gas-solid mixing and reaction in riser and downer under the influence of both co-current and counter-current injections are *** relative ozone concentration is used to reflect the location reaction extent and its radial nonuniformity index is proposed to compare the results in riser and *** is found that the jet influence zone in downer provides a relatively better environment for the mixing of feed jets with *** the riser,introduction of counter-current injections could improve the uniformity of gas-solid mixing in the initial contact region of feed with catalysts.

关键词： Riser Downer Gas-solid two-phase flow Jet

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Regulate electric double layer for one-step synthesize and modulate the morphology of(oxy)hydroxides

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Nano Research 2024年第5期17卷 3675-3683页

作者： Jiaxin Liu Yue Shi Yanli Gu Zheng Lv Liang Zhao Yu Yang Tianrong Zhan Jianping Lai Lei Wang State Key Laboratory Base of Eco-chemical engineering International Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong engineering Research Center for Marine environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

FeOOH have received considerable attention due to their natural abundance and *** the significant progress achieved,the one-step synthesis of integrated FeOOH is still a major ***,the current research on FeOOH catalyst still suffers from the unclear mechanism of controlling ***,density functional theory(DFT)calculations and X-ray photoelectron spectroscopy(XPS)demonstrated the strong electron-capturing and hydrogen absorption ability of Co in FeOOH,which further promotes the formation and stabilization of *** used a one-step electrodeposition method to synthesize Co introduced FeOOH integrated electrocatalyst and propose to introduce ions with different valence states to regulate the morphology of FeOOH by precise modulation of electric double layer(EDL)composition and *** prepared Co-FeOOH-K^(+)has a larger electrochemically active surface area(ECSA)(325 cm^(2))and turnover frequency(TOF)value(0.75 s^(-1)).In the electrochemical experiments of an alkaline anion exchange membrane electrolyzer,Co-FeOOH-K^(+)shows better oxygen evolution performance than commercial RuO_(2) under industrial production conditions and has good industrial application prospects.

关键词： integrated(oxy)hydroxides electrodeposition electric double layer(EDL) oxygen evolution reaction(OER) morphology regulation

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Bifunctional core–shell co-catalyst for boosting photocatalytic CO_(2) reduction to CH_(4)

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Nano Research 2024年第3期17卷 1259-1266页

作者： Fangxu Dai Mingming Zhang Jishu Han Zhenjiang Li Shouhua Feng Jun Xing Lei Wang Key Laboratory of Eco-chemical engineering Ministry of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China college of Materials Science and engineering Qingdao University of Science and TechnologyQingdao 266042China college of environment and Safety engineering Qingdao University of Science and TechnologyShandong Engineering Research Center for Marine Environment Corrosion and Safety ProtectionQingdao 266042China

Solar-light-driven CO_(2) reduction CO to CH_(4) and C2H6 is a complex process involving multiple elementary reactions and energy ***,achieving high CH_(4) activity and selectivity remains a significant ***,we integrate bifunctional Cu2O and Cu-MOF(MOF=metal-organic framework)core–shell co-catalysts(Cu2O@Cu-MOF)with semiconductor TiO_(2).Experiments and theoretical calculations demonstrate that Cu2O(Cu+facilitates charge separation)and Cu-MOF(Cu2+improves the CO_(2) adsorption and activation)in the core–shell structure have a synergistic effect on photocatalytic CO_(2) reduction,reducing the formation barrier of the key intermediate*COOH and**** photocatalyst exhibits high CH_(4) yield(366.0μmol·g^(-1)·h^(-1)),efficient electron transfer(3283μmol·g^(-1)·h^(-1))and hydrocarbon selectivity(95.5%),which represents the highest activity of Cu-MOF-based catalysts in photocatalytic CO_(2) reduction *** work provides a strategy for designing efficient photocatalysts from the perspective of precise regulation of components.

关键词： bifunctional co-catalyst core–shell photocatalytic CO_(2)reduction

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Process intensification for the synthesis and purification of battery-grade Li_(2)CO_(3)with microfluidics

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Particuology 2024年第7期90卷 106-117页

作者： Haodu Li Jie Zhang Lin Dai Le Du Jiqin Zhu The State Key Laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Battery-grade lithium carbonate(Li_(2)CO_(3))with a purity of higher than 99.5 wt%is of great importance as a high value-added lithium ***,influences of different reaction systems and process control on product purity remain ***,a membrane dispersion microreactor was used to enhance the mass transfer of preparation and purification processes in homogeneous and heterogeneous *** systems of Na_(2)CO_(3)–LiCl,NH_(4)HCO_(3)–LiCl,and NH_(3)·H_(2)O−CO_(2)−LiCl,CO_(2)purification based on carbonation and decomposition were *** Li_(2)CO_(3)purity was increased by the improvement of mixing *** carbonation time was reduced by 62.5%and 58.3%for the NH_(3)·H_(2)O−CO_(2)and CO_(2)purification systems,*** the two ammonia-based systems,Li_(2)CO_(3)particles with a purity of 99.7–99.8 wt%were one-step prepared with a size of 3–5μm,which also met the requirement of the battery-grade *** purity was further increased to 99.9 wt%by CO_(2)purification and LiHCO_(3)*** investigation could provide a feasible alternative for the controllable preparation of battery-grade Li_(2)CO_(3)in one or multiple steps.

关键词： Microfluidics Battery grade Li_(2)CO_(3) Process intensification High purity

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Unveiling the protective role of biofilm formation on the photoaging of microplastics

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Science China Technological Sciences 2024年第10期67卷 3067-3078页

作者： ZHANG HaiYu LIU Peng ZHANG JiaYu DAI JiaMin ZHANG XinRui ZHANG ZiXuan JIA HanZhong Key Laboratory of Plant Nutrition and the Agri-environment in Northwest China Ministry of AgricultureCollege of Natural Resources and EnvironmentNorthwest A&F University Key Laboratory of Organic Compound Pollution Control engineering School of Environmental and Chemical EngineeringShanghai University

In natural water, microplastics（MPs） inevitably undergo microbial colonization to form biofilm, while the effect of biofilm formation on the photoaging of MPs remains unknown. This study systematically investigated the photoaging behavior of disposable box-derived polypropylene（PPMPs） and polystyrene（PSMPs） mediated by formed biofilm in water. After incubating in Weihe water samples for 105 d, the biofilm was validated to form in PPMPs and PSMPs, with higher formation in PSMPs. In particular, biofilm formation inhibited the photoaging of PPMPs and PSMPs, with an 11.1% and 50.6% decrease in photooxidation compared to their virgin counterparts after 20 d of ultraviolet（UV） irradiation. Moreover, the photoaging route of MPs such as the reaction priority of functional groups（e.g., C–H, C=O, and benzene ring） was altered, indicating the important role of biofilm formation in the photoaging process of MPs. The protective effect of the biofilm was mainly caused by the role of optical light filters that absorbed UV energy by sacrificing themselves. Also, as the main attacker on MPs, the production of reactive oxygen species（ROS, mainly1O2and ·OH） was inhibited by biofilm, which was mainly responsible for the decreased photoaging of MPs. This study revealed the important role of biofilm in the photoaging process of MPs and suggested a higher resistance of（micro）plastics in natural water than that in the laboratory using pure MPs, which contributed to a deeper understanding of the environmental fate and pollution of MPs.

关键词： microplastics biofilm photoaging physical shielding reactive oxygen species

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