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

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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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Reconstruction of biomimetic ionic channels within covalent organic frameworks for ultrafast and selective uranyl capture

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Science China Chemistry 2024年第10期67卷 3423-3431页

作者： Cheng-Rong Zhang Xiao-Juan Chen Cheng-Peng Niu Cheng Meng Shun-Mo Yi Xin Liu Jia-Xin Qi Qiu-Xia Luo Ru-Ping Liang Jian-Ding Qiu State Key Laboratory of Nuclear Resources and environment East China University of Technology college of Chemistry and chemical engineering Nanchang University

The efficient extraction of uranium, as the primary component of nuclear energy, holds significant implications. Drawing inspiration from the charge interaction observed in biological ion channels, we encapsulated negatively charged polystyrene sulfonate(PSS) or sodium polystyrene carboxylate(PVBA) into the nanochannels of amidoxime functionalized covalent organic framework(COF-AO) in-situ to alter the cavity environment of COF-AO. The synthesized COF-AO-PSS and COF-AO-PVBA are used for ultra-fast and highly selective uranium recovery. The negatively charged PSS/PVBA was confined in the COF-AO channel providing the driving force for uranium transport and blocking other ions, thus creating a highly selective “uranium highway”. Additionally, introducing sulfonate groups or carboxyl groups into COF-AO offers supplementary coordination environments and weak interactions with uranium. Due to charge-assisted migration and various interaction mechanisms, both COF-AO-PSS and COF-AO-PVBA exhibit faster adsorption kinetics and higher selectivity compared to COF-AO alone. Their adsorption capacities are 3.8 times and 2.4 times that of COF-AO alone respectively which highlights the necessity for constructing biomimetic ion channels in uranium adsorption processes. This work presents a bionic adsorbent based on covalent organic frameworks(COFs) for the first time, overcoming environmental and equipment limitations associated with traditional photocatalysis and electrocatalysis methods for uranium capture, opening up new avenues for designing multifunctional materials that mimic biological systems.

关键词： covalent organic frameworks Uranium biomimetic ion-channels adsorption

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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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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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Two-dimensional C2N-based single-atom catalyst with complex microenvironment for enhanced electrochemical nitrogen reduction:A descriptor-based design

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Journal of Energy Chemistry 2024年第10期97卷 110-119页

作者： Enduo Dai Wei An Ruixian Guo Xugen Shi Yunyi Li Yibo Wang Mingming Liu college of Chemistry and chemical engineering Shanghai University of Engineering Science

The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild ***,we demonstrate that the descriptor Ω parameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst（SAC） for driving electrochemical nitrogen reduction（NRR）.Using twodimensional metal（M）-BxPySzNm@C2N as prototype SAC models,we reveal that*N2+（H++e-）→*N2H acts predominantly as the potential-limiting step（PLS） of NRR on M-B2P2S2@C2N and M-B1P1S1N3@C2N regardless of the distinction in coordination *** the 28 screened M active sites,with Ω values close to the optimal 4,M-B2P2S2@C2N(M=V（Ω=3.53）,Mo（Ω=5.12）,and W（Ω=3.92）) and M-B1P1S1N3@C2N(M=V（Ω=3.00）,Mo（Ω=4.34）,and W（Ω=3.32）) yield the lowered limiting potential（UL） as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR *** importantly,these SACs are located around the top of volcano-shape plot of ULversus Ω,re-validating Ω as an effective descriptor for accurately predicting the high-activity NRR SACs even with complex *** study unravels the relationship between active-site structure and NRR performance via the descriptor Ω,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules via σ-donation and π*-backdonation mechanism.

关键词： Descriptor DFT Electrocatalysis N2 reduction Single-atom catalyst

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Enhancement in the Hg^(0) oxidation efficiency and sulfur resistance of CuCl_(2)-modified MnO_(x)-CeO_(x) nanorod catalysts

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Journal of Zhejiang University-Science A(Applied Physics & engineering) 2024年第8期25卷 680-686页

作者： Shujie GAO Yongjin HU Zhichang JIANG Xiaoxiang WANG Dong YE Changxing HU college of Quality&Safety engineering China Jiliang UniversityHangzhou 310018China Key Laboratory of Biomass chemical engineering of Ministry of Education Institute of Industrial Ecology and EnvironmentCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China School of Mechatronics and Energy engineering Ningbo Tech UniversityNingbo 315100China

In this study,a series of CuCl_(2)-modified MnO_(x)-CeO_(x)nanorods were synthesized for the oxidation of Hg^(0).The addition of CuCl_(2)resulted in an enhancement in the catalyst’s Hg^(0)oxidation ability,and Hg^(0)oxidation efficiency reached>97%from 150 to 250°*** the MnO_(x)-CeO_(x)catalysts,Mn^(4+)played the role of the active species for Hg^(0)oxidization,but in the CuCl_(2)-doped catalysts Cl−also contributed to Hg^(0)oxidation,conferring the superior performance of these *** introduction of SO_(2) led to a decrease in the availability of Mn^(4+),and the Hg^(0)oxidation efficiency of MnO_(x)-CeO_(x)decreased from about 100%to about 78%.By contrast,CuCl_(2)-promoted samples maintained a Hg^(0)oxidation efficiency of about 100%during the SO_(2) deactivation cycle due to the high reactivity of Cl−.

关键词： Hg^(0)oxidation CuCl_(2)modification MnO_(x)-CeO_(x)nanorods Sulfur resistance O_(x)idation activity

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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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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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Long-term operation optimization of circulating cooling water systems under fouling conditions

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Chinese Journal of chemical engineering 2024年第1期65卷 255-267页

作者： Jiarui Liang Yong Tian Shutong Yang Yong Wang Ruiqi Yin Yufei Wang School of chemical engineering and environment China University of PetroleumBeijing102249China CHN Energy Xinjiang chemical Co. LTDUrumqi830092China college of Mechanical and Transportation engineering China University of PetroleumBeijing 102249China

Fouling caused by excess metal ions in hard water can negatively impact the performance of the circulating cooling water system(CCWS)by depositing ions on the heat exchanger's ***,the operation optimization of CCWS often prioritizes short-term flow velocity optimization for minimizing power consumption,without considering ***,low flow velocity promotes ***,it's crucial to balance fouling and energy/water conservation for optimal CCWS long-term *** study proposes a mixed-integer nonlinear programming(MINLP)model to achieve this *** model considers fouling in the pipeline,dynamic concentration cycle,and variable frequency drive to optimize the synergy between heat transfer,pressure drop,and *** optimizing the concentration cycle of the CCWS,water conservation and fouling control can be *** model can obtain the optimal operating parameters for different operation intervals,including the number of pumps,frequency,and valve local resistance *** experiments on cycle and environmental temperature reveal that as the cycle increases,the marginal benefits of energy/water conservation *** periods with minimal impact on fouling rate,energy/water conservation can be achieved by increasing the cycle while maintaining a low fouling ***,the proposed model has significant energy/water saving effects and can comprehensively optimize the CCWS through its incorporation of fouling and cycle optimization.

关键词： Computer simulation Circulating water system Fouling Concentration cycle Optimization Variable frequency drive

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