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Antimony oxides-protected ultrathin Ir-Sb nanowires as bifunctional hydrogen electrocatalysts

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Nano Research 2024年第3期17卷 1042-1049页

作者： Bingyan Xu Xuan Huang Shangheng Liu Zhiwei Hu Cheng-Wei Kao Ting-Shan Chan Hongbo Geng Ying Zhang Xiaoqing Huang Country State key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Max Planck Institute for Chemical Physics of solids Dresden 01187Germany “National Synchrotron Radiation Research Center” Hsinchu 30076TaiwanChina School of Materials Engineering Changshu Institute of TechnologyChangshu 215500China Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China

Developing electrocatalysts with fast kinetics and long-term stability for alkaline hydrogen oxidation reaction(HOR)and hydrogen evolution reaction(HER)is of considerable importance for the industrial production of green and sustainable ***,an ultrathin Ir-Sb nanowires(Ir-Sb NWs)protected by antimony oxides(SbO_(x))was synthesized as an efficient bifunctional catalyst for both HOR and HER under alkaline *** from the much higher mass activities of Ir-Sb nanowires than those of Ir nanowires(Ir NWs)and commercial Pt/C,the SbO_(x) protective layer also contributes to the maintenance of morphology and anti-CO poisoning ability,leading to the long-term cycling performance in the presence of ***,the Ir-Sb NW/SbO_(x) exhibits the highest catalytic activities,which are about 3.5 and 4.8 times to those of Ir NW/C and commercial Pt/C toward HOR,*** work provides that the ultrathin morphology and H_(2)O-occupied Sb sites can exert the intrinsic high activity of Ir and effectively optimize the absorption of OH*both in alkaline HER/HOR electrolysis.

关键词： Ir nanowire amorphous antimony oxides bifunctional mechanism hydrogen evolution reaction hydrogen oxidation reaction

Advanced Materials for NH_(3)Capture:Interaction Sites and Transport Pathways

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Nano-Micro Letters 2024年第11期16卷 119-155页

作者： Hai‑Yan Jiang Zao‑Ming Wang Xue‑Qi Sun Shao‑Juan Zeng Yang‑Yang Guo Lu Bai Ming‑Shui Yao Xiang‑Ping Zhang key laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190People’s Republic of China School of Future Technology University of Chinese Academy of SciencesBeijing 100049People’s Republic of China China University of Petroleum Beijing 102249People’s Republic of China Institute for Integrated Cell‑Material Sciences(iCeMS) Kyoto UniversitySakyo‑KuYoshidaKyoto 606‑8501Japan

Ammonia(NH3)is a carbon-free,hydrogen-rich chemical related to global food safety,clean energy,and environmental *** an essential technology for meeting the requirements raised by such issues,NH3 capture has been intensively explored by researchers in both fundamental and applied *** four typical methods used are(1)solvent absorption by ionic liquids and their derivatives,(2)adsorption by porous solids,(3)abadsorption by porous liquids,and(4)membrane *** in the development of advanced materials for NH3 capture,we conducted a coherent review of the design of different materials,mainly in the past 5 years,their interactions with NH3 molecules and construction of transport pathways,as well as the structure–property relationship,with specific examples ***,the challenges in current research and future worthwhile directions for NH3 capture materials are proposed.

关键词： Ammonia capture Solvents Porous solids Porous liquids Membranes

Experimental investigation of bed-to-wall heat transfer in fluidized beds of a Geldart B sorbent particle under a full spectrum of fluidization regime

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Particuology 2024年第10期93卷 235-246页

作者： Chenhuan Xu Yongmin Zhang Liang Wang Yiming Zhang Tianlei Yang Feng Qiu Cenfan Liu Shuai Jiang Ke Dong State key laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China Beijing DERUNCHEN Environmental Protection Technology Co. LtdBeijing100022China key laboratory of Special Equipment Safety and Energy-saving for State Market Regulation China Special Equipment Inspection and Research InstituteBeijing100029China

Fluidization technology has been used in CO_(2) capture processes, the successful design and operation of the heat exchangers involved in this process require much information on the bed-to-wall heat transfer of the sorbent particles in fluidized states. In this study, the bed-to-wall heat transfer coefficient (h) of a solid amine sorbent was measured by a heat transfer probe in a large-scale circulating fluidized bed cold model unit, where full spectrum of fluidization regimes can be realized. The corresponding hydrodynamic signals were also studied by pressure sensors and optical fiber probes to further explain the newly discovered phenomenon. The results show that in a dense bed, due to the counterbalanced effect of time fraction of packet and packet renewal frequency, h of the Geldart B particle reaches a peak within the bubbling fluidized regime, and the radial distribution of h are opposite in bubbling and turbulent fluidized regimes. In a fast fluidization regime, gas convection becomes the dominant factor affecting h when the solids holdup is low enough. Correlations were provided or recommended to guide the design of heat exchangers in the fluidized bed CO_(2) capture processes.

关键词： Bed-to-wall heattransfer Solid amine sorbent Geldart B particle Full spectrum of fluidization regime Correlation

Selective CO_(2)Electroreduction to Multi-Carbon Products on organic-Functionalized CuO Nanoparticles by Local Micro-Environment Modulation

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Nano-Micro Letters 2024年第12期16卷 120-132页

作者： Shan Ren Xi Cao Qikui Fan Zhimao Yang Fei Wang Xin Wang Licheng Bai Jian Yang Materials Interfaces Center Shenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055GuangdongPeople’s Republic of China key laboratory of Functional Molecular solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002AnhuiPeople’s Republic of China School of Physics Xi’an Jiaotong UniversityXi’an 710049ShaanxiPeople’s Republic of China College of Materials Science and Engineering Shenzhen UniversityShenzhen 518071GuangdongPeople’s Republic of China

Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO_(2)/CO concentration at the *** upon this approach,we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CO_(2)RR to C_(2+)in a neutral *** CuO nanoparticles coated with hexaethynylbenzene organic molecules(HEB-CuO NPs),a remarkable C_(2+)Faradaic efficiency of nearly 90%was achieved at an unprecedented current density of 300 mA cm^(-2),and a high FE(>80%)was maintained at a wide range of current densities(100-600 mA cm^(-2))in neutral environments using a flow ***,in a membrane electrode assembly(MEA)electrolyzer,86.14%FEC2+was achieved at a partial current density of 387.6 mA cm^(-2)while maintaining continuous operation for over 50 h at a current density of 200 mA cm^(-2).In-situ spectroscopy studies and molecular dynamics simulations reveal that reducing the coverage of coordinated K⋅H2O water increased the probability of intermediate reactants(CO)interacting with the surface,thereby promoting efficient C-C coupling and enhancing the yield of C_(2+)*** advancement offers significant potential for optimizing local micro-environments for sustainable and highly efficient C_(2+)production.

关键词： CO_(2)electroreduction to C_(2+) Neutral electrolyte organic-functionalized CuO nanoparticles Local micro-environment

A MOF built on 8-connected Y3 nodes demonstrates simultaneous reverse adsorptive separation: ethane over ethylene and propane over propylene

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Science China Chemistry 2024年第11期67卷 3657-3661页

作者： Lu-Lu Ma Jiaqi Liu Kang Zhou Zixuan Cao Jiafeng Miao Guo-Ping Yang Yao-Yu Wang Jing Li Hao Wang key laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education Shaanxi Key Laboratory of PhysicoInorganic Chemistry College of Chemistry & Materials Science Northwest University Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University Shenzhen Senior High School Department of Chemistry and Chemical Biology Rutgers University

Selective adsorption of paraffins over olefins（mostly C2 and C3） by porous solids could offer tremendous advantages for the purification of olefins, which is, however, challenging as it has stringent requirements on the pore dimensions and pore surface chemistry of the adsorbent. We report here a metal-organic framework（MOF） with novel topology, Y3（μ3-OH）(TCMPB)2(denoted as HIAM-316, TCMPB4-= 1,2,4,5-tetra（4-carboxy-3-methylphenyl）benzene), which shows reversed separation of C2H6/C2H4and C3H8/C3H6simultaneously. The ideal adsorbed solution theory（IAST） selectivities for equimolar binary mixtures of C2H6/C2H4and C3H8/C3H6were calculated to be 1.67 and 1.23 at 1 bar and 298 K for HIAM-316. Its capability of removing paraffines from paraffin/olefin mixtures is validated by breakthrough measurements. Molecular simulations reveal that the preferential adsorption of paraffins over olefins by HIAM-316 may be attributed to the abundant carboxylate oxygen atoms along its channel.

关键词： metal-organic framework adsorption separation

Coupling of BiOCl Ultrathin Nanosheets with Carbon Quantum Dots for Enhanced Photocatalytic Performance

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Transactions of Tianjin University 2024年第3期30卷 211-220页

作者： Pin Song Xiaoyu Fang Wei Jiang Yuyang Cao Daobin Liu Shiqiang Wei Jun Du Lang Sun Lei Zhao Song Liu Yuzhu Zhou Jun Di Chade Lv Bijun Tang Jiefu Yang Tingting Kong Yujie Xiong key laboratory of Functional Molecular solids Ministry of EducationAnhui Engineering Research Center of Carbon NeutralityCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241000China National Synchrotron Radiation laboratory CAS Center for Excellence in NanoscienceSchool of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230029China School of Chemistry and Chemical Engineering National Special Superfi ne Powder Engineering Research CenterNanjing University of Science and TechnologyNanjing 210094China MIIT key laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China School of Materials Science&Engineering Nanyang Technological UniversitySingapore 639798Singapore

Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution *** novel materials with outstanding photocatalytic activities has become a research hotspot in this *** this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal *** photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light *** with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of ***,photocatalytic N_(2)reduction performance was significantly improved after introducing *** 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites.

关键词： Carbon quantum dots BiOCl Rhodamine B Tetracycline Photocatalysis

Alkyl-thiophene-alkyl linkers to construct double-cable conjugated polymers for single-component organic solar cells

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Chinese Chemical Letters 2024年第1期35卷 542-546页

作者： Wenbin Lai Safakath Karuthedath Chengyi Xiao Lei Meng Frédéric Laquai Weiwei Li Yongfang Li Beijing National laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Beijing Advanced Innovation Center for Soft Matter Science and Engineering&State key laboratory of organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China King Abdullah University of Science and Technology(KAUST) KAUST Solar Center(KSC)Physical Sciences and Engineering Division(PSE)Material Science and Engineering Program(MSE)Thuwal 23955-6900Kingdom of Saudi Arabia University of Chinese Academy of Sciences Beijing 100049China Institute of Materials Research Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China

In this work,semirigid linkers of the alkyl-thiophene-alkyl structure are developed to construct double-cable *** alkyl units,propyl(C3H6),hexyl(C6H12),and dodecyl(C12H24),are applied as semirigid linkers,yielding three double-cable polymers:PBC6-T,PBC12-T,and PBC24-T,***12-T which uses C6H12-thiophene-C6H12 linkers is found to exhibit the best device efficiency of 5.56%,while PBC6-T and PBC24-T with shorter or longer linkers yield device efficiencies of only 2.65%and 1.09%in single-component organic solar cells(SCOSCs).Further studies reveal that PBC12-T exhibits higher crystallinity and improved charge transport,resulting in better *** work provides an approach to construct double-cable conjugated polymers with long alkyl linkers,and it shows the importance of the linker length for the photovoltaic performance of SCOSCs.

关键词： Double-cable conjugated polymer Single-component organic solar cell Crystallinity Semirigid linkers Alkyl-thiophene-alkyl

Hydrodynamics and OCM reaction performance in a bubbling fluidized bed reactor and a riser reactor

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Particuology 2024年第3期86卷 188-204页

作者： Min Cai Shuangzhu Kong Sheng Chen Mengxi Liu Chunxi Lu State key laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China China Special Equipment Inspection and Research Institute Beijing102249China

The reasonable reactor design is of great importance for increasing the C_(2) yield(C2H4 and C2H6)of the oxidative coupling of methane(OCM),and the OCM reactor should remove the heat released in reactions quickly and efficiently and minimize the consecutive reaction of ethylene to carbon *** fluidized bed reactor is characterized by excellent heat transfer,superior mass transport,and large handling capacity,while fewer studies focused on large-scale fluidized bed reactors for the OCM ***,large cold-model experiments and computational fluid dynamics simulations were conducted to investigate hydrodynamics and the OCM reaction performance in a large-scale bubbling fluidized bed(BFB)and a large-scale *** the BFB reactor,consecutive reactions of ethylene are acute because of the strong gas back-mixing,high solids holdup,and non-uniform solids *** the consecutive reactions of ethylene are negligible due to the plug flow structure and low solids holdup in the riser ***,both reactors can achieve isothermal operation for the OCM *** C_(2) selectivity of 45.4% and C_(2) yield of 21.1% are obtained in the riser reactor,increasing by 20.3% and 5.8% individually than that in the BFB *** study provides useful information and reference to the OCM reactor designandcommercialization.

关键词： Oxidative coupling of methane Bubbling fluidized bed reactor Riser reactor Hydrodynamics Isothermal operation

Toward a rapid and convenient nanoplastic quantification method in laboratory-scale study based on fluorescence intensity

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Frontiers of Environmental Science & Engineering 2024年第5期18卷 117-126页

作者： Ruiqi Yan Sen Lin Qian Ding Lei Zhang Xia Yu Wentao Zhao Qian Sui State Environmental Protection key laboratory of Environmental Risk Assessment and Control on Chemical Process School of Resources and Environmental EngineeringEast China University of Science and TechnologyShanghai200237China State key laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

The thorough investigation of nanoplastics(NPs)in aqueous environments requires efficient and expeditious quantitative analytical methods that are sensitive to environmentally relevant NP concentrations and convenient to *** analysis-based quantitative methods have been acknowledged as effective and rapid approaches for quantifying NP concentrations in laboratory-scale ***,we compared three commonly used optical response indicators,namely fluorescence intensity(FI),ultraviolet absorbance,and turbidity,to assess their performance in quantifying ***,orthogonal experiments were conducted to evaluate the influence of various water quality parameters on the preferred indicator-based quantification *** results revealed that FI exhibits the highest correlation coefficient(>0.99)with NP ***,the limit of quantification(LOQ)for various types of NPs is exceptionally low,ranging from 0.0089 to 0.0584 mg/L in ultrapure water,well below environmentally relevant *** variations in water quality parameters such as pH,salinity,suspended solids(SS),and humic acid,a robust relationship between detectable FI and NP concentration was ***,an increased matrix,especially SS in water samples,results in an enhanced LOQ for ***,the quantitative method remains applicable in real water bodies,especially in drinking water,with NP LOQ as low as 0.0157–0.0711 mg/*** exceeds the previously reported detectable concentration for 100 nm NPs at 40µg/mL using surface-enhanced Raman *** study confirms the potential of FI as a reliable indicator for the rapid quantification of NPs in aqueous environments,offering substantial advantages in terms of both convenience and cost-effectiveness.

关键词： Nanoplastic quantification Fluorescence intensity Drinking water Limit of quantification(LOQ) Matrix effects