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Compositional evolution for mixed aerosols containing gluconic acid and typical nitrate and the effect of multiply factors on hygroscopicity

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Journal of Environmental Sciences 2024年第5期139卷 206-216页

作者： Yue Zhu Shufeng Pang Yunhong Zhang school of Chemistry and chemical engineering Beijing Institute of TechnologyBeijing 100081China

The aging process of atmospheric aerosols usually leads to a mixture of inorganic salts and organic compounds of anthropogenic origin.In organic compounds,polyhydroxy organic acids are important components,however,the study on composition and hygroscopic properties of the mixture containing inorganics and polyhydroxy organic acids is scanty.In this study,gluconic acid,the proxy of polyhydroxy organic acids,is mixed with the representative nitrate(Mg(NO_(3))_(2),Ca(NO_(3))_(2))to form aerosols.ATR-FTIR and optical microscopy are employed to study the component changes and hygroscopicity as a function of relative humidity.As relative humidity fluctuates,the FTIR-ATR spectra display that the internal mixed gluconic acid(CH_(2)(CH)_(4)(OH)_(5)COOH)and nitrate can react to release acidic gases,forming relevant gluconate and further affecting the hygroscopicity.The specific presentation is particles cannot be recovered to their original size after the dehydration-hydration process and there will be some disparities in GF for mixed particles.For the gluconic acid-Ca(NO_(3))_(2)/Mg(NO_(3))_(2)mixtures with molar ratios of 1:1,higher degree of reaction resulting in the production of large amounts of gluconate should be responsible to the lower hygroscopicity compared to ZSR model.For 1:2 gluconic acid-nitrate mixed systems(with higher nitrate content),the hygroscopicity of mixtures are higher than the ZSR prediction.A possible reason could be‘salt-promoting effect’on the organic fractions of the surplus inorganic salt in the mixture.These data can improve the chemical composition list evaluation,in turn hygroscopic properties and phase state of atmospheric aerosol,and then the climate effect.

关键词： Hygroscopicity Gluconic acid Reaction ZSR simulation Size growth factors

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High adsorption selectivity of activated carbon and carbon molecular sieve boosting CO_(2)/N_(2) and CH_(4)/N_(2) separation

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Chinese Journal of chemical engineering 2024年第3期67卷 282-297页

作者： Siang Chen Wenling Wu Zhaoyang Niu Deqi Kong Wenbin Li Zhongli Tang Donghui Zhang The Research Center of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 kPa.The experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric heat.Both the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular sieve.Moreover,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) separation.The study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.

关键词： Activated carbon Carbon molecular sieve Adsorbent evaluation Adsorption equilibrium and kinetics Heat of adsorption Selectivity

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Constructing core@shell structured photothermal nanosphere with thin carbon layer confined Co-Mn bimetals for pollutant degradation and solar interfacial water evaporation

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Rare Metals 2024年第4期43卷 1686-1701页

作者： Hong-Yang Zhu Meng-Ting Liu Gang Wang Rong-Rong Du Hong-Yao Zhao Hao Lu Shi-Qi Yang Sheng Tang Zeng-Jing Guo Jun Yang Cheng-Zhang Zhu Fu Yang school of Environmental and chemical engineering Jiangsu University of Science and Technology school of Chemistry and chemical engineering Liaocheng University school of Material Science and engineering Jiangsu University of Science and Technology school of Environmental Science and engineering Nanjing Tech University

Photothermal material applied in environmental governance has attracted growing attention.By combining the Stober method and dopamine-triggered coating strategy,Co-Mn precursor was in situ incorporated into the poly dopamine（PDA） layer over the surface of silica cores.Afterwards,a unique photothermal nanosphere with SiO2core and thin carbon layer and dual Co-Mn oxides shell was allowed to form by sequential heat treatment in the inert atmosphere（SiO2@CoMn/C）.The bimetallic fraction of Co/Mn in the carbon layer and post-treatment calcination temperature was comprehensively tuned to optimize the peroxymonosulfate（PMS） activation performance of the catalyst.The state of bimetallic species was studied including their physical distribution,chemical valence,and interplay by various characterizations.Impressively,Co oxides appear as dominant monodispersed nanoparticles（～ 10 nm）,while Mn with cluster-like morphology is observed to uniformly distribute over thin-layer carbon and adhered to the surface of SiO2nanospheres（～ 250 nm）.The calcined temperature could tune the oxidized state of Co species,leading to the optimization of the catalytic performance of introduced dual metal species.As a result,this obtained optimal catalyst integrated the advantages of exposed bimetallic CoMn species and N-doped thin carbon to deliver excellent catalytic PMS activation performance and photothermal synergetic catalytic mineralization ability for diversiform pollutants.Further reactions condition controls and anion interference studies were conducted to identify the adaptability of the optimal catalyst.Moreover,the application of solar-driven interfacial water evaporation using optimal SiO2@Co3Mn1/C-600 catalyst was explored,showing a high water evaporation rate of 1.48 kg·m-2·h-1and an efficiency of 95.2%,further revealing a comprehensive governance functionality of obtained material in the complex pollution condition.

关键词： Photothermal Peroxymonosulfate (PMS) activation Bimetallic synergy Water evaporation Advanced oxidation process

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Transient synthesis of carbon-supported high-entropy alloy sulfide nanoparticles via flash Joule heating for efficient electrocatalytic hydrogen evolution

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Nano Research 2024年第4期17卷 3379-3389页

作者： Yuntian Liao Rongtao Zhu Wenjun Zhang Haiyang Zhu Yang Sun Jiale Chen Zhenhua Dong Ronghuan Lv school of chemical engineering and technology China University of Mining and TechnologyXuzhou 221116China

High entropy alloys(HEA)are frequently employed as catalysts in electrocatalytic hydrogen evolution.However,the traditional high entropy alloy synthesis methods are time-consuming,energy-intensive,and environmentally polluting,which limits their application in the hydrogen evolution reaction(HER).This study leveraged the capabilities of flash Joule heating(FJH)to synthesize carbon-supported high-entropy alloy sulfide nanoparticles(CC-S-HEA)on carbon cloth(CC)with good self-standing properties within 300 ms.The carbon thermal shock generated by the Joule heating could pyrolyze the sulfur source into gas,resulting in numerous pore structures and defects on CC,forming an S-doped carbon substrate(CC-S).Then the S atoms were used to stably anchor the metal atoms on CC-S to form high-density uniformly dispersed HEA particles.The electrochemical test results demonstrated that CC-S-HEA prepared at 60 V flash voltage had HER performance comparable to Pt/C.The density functional theory(DFT)calculation indicated that the S atoms on CC-S accelerated the electron transfer between the carbon substrate and HEA particles.Moreover,the unique electronic structure of CC-S-HEA was beneficial to H*adsorption and promoted catalytic kinetics.The simplicity and versatility of FJH synthesis are of great significance for optimizing the synthesis of HEA and improving the quality of HEA products,which provides a broad application prospect for the synthesis of nanocatalysts with efficient HER performance.

关键词： high entropy alloy flash Joule heating carbon thermal shock hydrogen evolution reaction density functional theory

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Combined effects of sea urchin-like structure and mixed Cu^(+)/Cu^(0)states on promoting C_(2)formation in electrocatalytic CO_(2)reduction

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Frontiers of chemical Science and engineering 2024年第3期18卷 63-73页

作者： Mengqing Shan Dongsheng Lu Jiatong Dong Shen Yan Jinyu Han Hua Wang Collaborative Innovation Center of chemical Science and engineering Key Laboratory for Green Chemical Technology of the Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300354China

Surface engineering and Cu valence regulation are essential factors in improving the C_(2)selectivity during the electrochemical reduction of CO_(2).Herein,we present a sea urchin-like CuO/Cu_(2)O catalyst derived from rhombic dodecahedra Cu_(2)O through one-step oxidation/etching method where the mixed Cu^(+)/Cu^(0)states are formed via in situ reduction during electrocatalysis.The combined effects of the morphology and the mixed Cu^(+)/Cu^(0)states on C–C coupling are evaluated by the Faradaic efficiency of C_(2)and the C_(2)/C1 ratio obtained in an H-cell.R-Cu^(O)/Cu_(2)O exhibited 49.5%Faradaic efficiency of C_(2)with a C_(2)/C1 ratio of 3.1 at−1.4 V vs.reversible hydrogen electrode,which are 1.5 and 3.2 times higher than those of R-Cu_(2)O,respectively.Using a flow-cell,68.0%Faradaic efficiency of C_(2)is achieved at a current density of 500 mA·cm^(−2).The formation of the mixed Cu^(+)/Cu^(0)states was confirmed by in situ Raman spectra.Additionally,the sea urchin-like structure provides more active sites and enables faster electron transfer.As a result,the excellent C_(2)production on R-CuO/Cu_(2)O is primarily attributed to the synergistic effects of the sea urchin-like structure and the stable mixed Cu^(+)/Cu^(0)states.Therefore,this work presents an integrated strategy for developing Cu-based electrocatalysts for C_(2)production through electrochemical CO_(2)reduction.

关键词： CO_(2)electrolysis sea urchin-like structure Cu^(+)/Cu^(0) C_(2)products

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Optimization on crystallization process of the magnetic core lysozyme

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Particuology 2024年第4期87卷 106-113页

作者： Lixia Hou Chunxiao Qu Min Su Zhihan Liang Qi Hao school of chemical engineering Hebei University of TechnologyTianjin300130China

The continuous growth of the biomedical market highlights the significance of improvement in the ef-ficiency of batch production for protein drug crystals.Herein,we investigated the effect of polymer-modified Fe_(3)O_(4) nanoparticles on lysozyme(Lys)crystallization at different conditions,using function-alized Fe_(3)O_(4) magnetic nanoparticles(Polymer C@Fe_(3)O_(4))as nucleation agents.The study revealed that the surface charge density of Polymer C@Fe_(3)O_(4) was highest at a modification mass ratio of Fe_(3)O_(4) to Polymer C is 8∶3.This ratio facilitates the augmentation of electrostatic interaction and the promotion of crys-tallization.By adding 15%of the PolymerC@Fe_(3)O_(4) prepared from Fe_(3)O_(4) with an average particle size of 150 nm,the magnetic core lysozyme(M-Lys)crystals with an average particle size of 11.08μm,narrow size distribution,and regular morphology were obtained in a yield of 82.42%within 60 min.

关键词： Protein Crystallization Magnetic particle Lysozyme

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Effectively improving the extreme-pressure capacity of a class of intercalated zirconium phosphate materials

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Science China(Technological Sciences) 2024年第3期67卷 753-764页

作者： NIU WenXing ZHAO XinRui YUAN Min HOU ZhiGuo LIU Lei XU Hong DONG JinXiang Shanxi Key Laboratory of chemical Product engineering Cllege of Chemical Engineering and TechnologyTaiyuan University of TechnologyTaiyuan 030024China school of chemical and Environmental engineering Pingdingshan UniversityPingdingshan 467000China

We studied different long-chain ammonium ions intercalated zirconium phosphate α-ZrP, methylamine intercalated ZrP(MAZrP), tetramethylammonium hydroxide intercalated ZrP(TMAH-ZrP), dodecyltrimethylammonium bromide intercalated ZrP(DTAB-ZrP), and stearyl trimethyl ammonium bromide intercalated ZrP(STAB-ZrP) as grease co-additives in combination with isobutylene sulfide(SIB). The grease with co-additives displayed excellent extreme-pressure and anti-wear performance.Moreover, the combination of the longest chain ammonium ion intercalated zirconium phosphate, STAB-ZrP/SIB, had the best tribological properties. In comparison to α-ZrP, the advantage of STAB-ZrP was that it did not form a large area of the dense physical film like α-ZrP on the worn surface, but rather gave the SIB a chance to contact with the fresh metal surface to generate a chemical film. Therefore, the sub-micron physical film and nanoscale chemical film always exist side by side on the contact surface during the friction process. This intercalated α-ZrP/SIB additive has great potential for use in harsh operating conditions.

关键词： intercalatedα-ZrP/SIB physical film chemical film tribological properties

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Kinetics and mechanism of propylene hydro-oxidation to acrolein on Au catalysts

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Nano Research 2024年第1期17卷 354-363页

作者： Wei Du Zhihua Zhang Nan Song Xuezhi Duan Xinggui Zhou State Key Laboratory of chemical engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Propylene epoxidation by H_(2)and O_(2)to propylene oxide(PO)over the Au-Ti bifunctional catalysts,as an ideal reaction for PO production,has attracted great interest.Revealing the mechanism of acrolein formation is of great importance for understanding the mechanism of molecular oxygen activation and the formation of hydroperoxo species on the Au sites.Here,we investigate the reaction mechanism of propylene oxidation to acrolein on the Au/uncalcined TS-1(Au/TS-1-B)catalyst through a combination of multiple characterization,H_(2)/D_(2)exchange,kinetics experiment,and modeling.The Ti sites are found to be non-essential to acrolein formation.Moreover,the acrolein formation on the Au/TS-1-B catalyst is confirmed to be promoted by H_(2)through hydroperoxo species formation,which includes two main steps:propylene dehydrogenation to*C_(3)H_(5)with the aid of*OOH species,and*C_(3)H_(5)oxidation by*OOH to acrolein.The latter step is determined to be the rate-determining step because the corresponding kinetics model gives the best description for experimental results.This work not only provides kinetics insights for the propylene hydro-oxidation to acrolein on the Au-Ti bifunctional catalysts,but also facilitates the rational design of Au catalysts with high activity and selectivity in the direct propylene epoxidation with H_(2)and O_(2).

关键词： kinetics mechanism gold acrolein hydro-oxidation

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NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu State Key Laboratory Base of Eco-chemical engineering College of chemical engineering Qingdao University of Science and TechnologyQingdao266042China Key Laboratory for Green chemical technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive attention.However,the low activity,insufficient selectivity and high cost of catalysts have been the bottlenecks.Herein,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se deficiency.The cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V vs.reversible hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V vs.RHE),and the average electron transfer number is about 2.3.Furthermore,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V vs.RHE,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

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Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Journal of Energy Chemistry 2024年第8期95卷 20-28页

作者： Siyi Hou Xuedan Song Chang Yu Jiangwei Chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State Key Lab of Fine chemicals Liaoning Key Lab for Energy Materials and Chemical Engineering Frontier Science Center for Smart Materials School of Chemical EngineeringDalian University of Technology Liaoning Key Lab for Energy Materials and chemical engineering Frontier Science Center for Smart Materials School of Chemistry Dalian University of Technology State Key Laboratory of chemical Resource engineering College of Chemical Engineering Beijing University of Chemical Technology

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon materials. However, the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging task. Herein, the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center calculations. To experimentally verify this, the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P), subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO) via π-π interactions. The multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-ordered π electron delocalization system as conductive network. The defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%, superior to the Pt reference(7.97%). Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates, thus enhancing the electrocatalytic activity of the catalyst. This work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Carbon quantum dots Defect engineering Electrocatalytic activity Pentagon carbon Triiodide reduction

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