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Siliceous mesocellular foam supported Cu catalysts for promoting non-thermal plasma activated CO_(2) hydrogenation toward methanol synthesis

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Frontiers of chemical Science and engineering 2024年第7期18卷 55-65页

作者： Yi Chen Shaowei Chen Yan Shao Cui Quan Ningbo Gao Xiaolei Fan Huanhao Chen State Key Laboratory of Materials-Oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China School of environmental Science and engineering Nanjing Tech UniversityNanjing 211816China School of Energy and Power engineering Xi’an Jiaotong UniversityXi’an 710049China Department of chemical engineering School of EngineeringThe University of ManchesterManchester M139PLUK Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute University of Nottingham Ningbo ChinaNingbo 315048China Institute of Wenzhou Zhejiang UniversityWenzhou 325006China

Electrified non-thermal plasma (NTP) catalytic hydrogenation is the promising alternative to the thermal counterparts, being able to be operated under mild conditions and compatible with green electricity/hydrogen. Rational design of the catalysts for such NTP-catalytic systems is one of the keys to improve the process efficiency. Here, we present the development of siliceous mesocellular foam (MCF) supported Cu catalysts for NTP-catalytic CO_(2) hydrogenation to methanol. The findings show that the pristine MCF support with high specific surface area and large mesopore of 784 m2·g−1 and ~8.5 nm could promote the plasma discharging and the diffusion of species through its framework, outperforming other control porous materials (viz., silicalite-1, SiO_(2), and SBA-15). Compared to the NTP system employing the bare MCF, the inclusion of Cu and Zn in MCF (i.e., Cu1Zn1/MCF) promoted the methanol formation of the NTP-catalytic system with a higher space-time yield of methanol at ~275 μmol·g_(cat)^(−1)·h^(−1) and a lower energy consumption of 26.4 kJ^(−1)·mmol_(CH_(3)OH)^(-1) (conversely, ~225 μmol·g_(cat)^(−1)·h^(−1) and ~71 kJ^(−1)·mmol_(CH_(3)OH)^(-1), respectively, for the bare MCF system at 10.1 kV). The findings suggest that inclusion of active metal sites (especially Zn species) could stabilize the CO_(2)/CO-related intermediates to facilitate the surface reaction toward methanol formation.

关键词： non-thermal plasma(NTP)catalysis Cu catalyst CO_(2)hydrogenation methanol siliceous mesocellular foam(MCF)

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Ni/Co bimetallic organic frameworks nanospheres for highperformance electrochemical energy storage

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Nano Research 2024年第6期17卷 5122-5130页

作者： Jianru Guan Minlu Liu Limin Zhu Jiamei Wang Qing Han Xiaoxia Yang Weibo Hua Lingling Xie Xiaoyu Cao School of Chemistry and chemical engineering Key Laboratory of High Specific Energy Materials for Electrochemical Power Sources of Zhengzhou CityHenan University of TechnologyZhengzhou 450001China School of chemical engineering and Technology Xi’an Jiaotong UniversityXi’an 710049China School of environmental engineering Henan University of TechnologyZhengzhou 450001China

In addition to their many well-known advantages(e.g.,ultra-high porosity,good pore size distribution,easy functionalization,and structural tolerability),metal-organic frameworks(MOFs)are a new class of advanced functional ***,their backbones are highly susceptible to deformation after exposure to acidic or alkaline *** a result of lithium-ion batteries embedding or detaching directly from MOFs,they irreversibly *** a result,they fail to maintain their electrochemical *** factors have hindered the development of MOFs as direct electrode materials,making the design of MOF materials with controlled morphology and stable dimensions a new *** this study,we adopted a versatile and effective method to synthesize a novel MOF material(NiCo-BP(BP=BTC/phen and BTC=1,3,5-benzenetricarboxylic acid))using the rigid ligands 1,10-phenanthroline and homobenzotrizoic acid,and the emergence of the Ni-O/N and Co-O/N coordination layers was observed by extended X-ray absorption fine structure(EXAFS)tests,indicating that Ni and Co were coordinated with heterocyclic N-given atoms to form a stable p-πconjugated ***,the metal-ion is attached to the carboxylic acid ligand on the other side,making the metal-organic skeleton complete and *** nanosphere structure of NiCo-BP(~400 nm)allows for full exposure and utilisation of the active sites,especially the Ni,Co,and phenanthroline units,and exhibit impressively high specific capacity and cycling *** a high current density of 1.0 A·g^(−1),a high discharge specific capacity of 631.6 mAh·g^(−1)was obtained after 1000 *** co-participation of two organic ligands in the coordination is in accordance with the theory of soft and hard acids and bases,which contributes to the ability of the material to maintain a high capacity in cycling as well as its cyclic stability.

关键词： lithium-ion batteries metal organic frame electrochemical energy storage dual ligand hard-soft-acid-base

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Defect-induced synthesis of nanoscale hierarchically porous metal-organic frameworks with tunable porosity for enhanced volatile organic compound adsorption

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Nano Materials Science 2024年第4期6卷 467-474页

作者： Kuan Liang Weibiao Guo Linmei Li Huidong Cai Haiqi Zhang Jingjing Li Feng Xu Jian Yan Daofei Lv Hongxia Xi Chongxiong Duan Guangdong Provincial Key Laboratory of Intelligent Food Manufacturing Foshan University School of Materials Science and Hydrogen engineering Foshan University School of Chemistry and chemical engineering South China University of Technology School of environmental and chemical engineering Foshan University

Nanoscale hierarchically porous metal-organic frameworks （NH-MOFs） synergistically combine the advantages of nanoscale MOFs and hierarchically porous MOFs,resulting in remarkable characteristics such as increased specific surface area,greater porosity,and enhanced exposure of active ***,nanoscale hierarchically porous UIO-66 （UIO-66＿X） was synthesized using a defect-induced strategy that employed ethylene diamine tetraacetic acid （EDTA） as a *** introduced EDTA occupies the coordination sites of organic ligands,promoting the formation and growth of UIO-66 crystal nuclei and inducing defects during *** as-synthesized UIO-66＿X crystals exhibit a uniform distribution with an average size of approximately 100 *** addition,the total pore volume attains a remarkable value of 0.95 cm3g-1,with mesopores constituting 36.8%of the ***,the porosities of UIO-66＿X can be easily tuned by controlling the molar ratio of EDTA/Zr4+.In addition,the as-synthesized UIO-66＿X exhibits excellent adsorption capacities for n-hexane (344 mg g-1) and pxylene (218 mg g-1),which are 44.5%and 27.5%higher than those of conventional UIO-66,***,the adsorption behavior of n-hexane and p-xylene molecules in UIO-66＿X was investigated using density functional theory simulations.

关键词： Nanoscale hierarchically porous MOFs Tunable porosities Enhanced VOC adsorption

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Hydroxyl radical production by abiotic oxidation of pyrite under estuarine conditions:The effects of aging,seawater anions and illumination

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Journal of environmental Sciences 2024年第1期135卷 715-727页

作者： Ruixue Liu Yinshun Dai Yucheng Feng Shiwen Sun Xiaodong Zhang Chunjiang An Shan Zhao Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityQingdao 266237China Department of Building Civil and Environmental EngineeringConcordia UniversityMontrealQC H3G 1M8Canada

Pyrite is widely distributed in estuarine sediments as an inexpensive natural Fenton-like reagent,however,the mechanism on the hydroxyl radical(HO^(·))production by pyrite under estuarine environmental conditions is still poorly *** batch experiments were performed to investigate the effects of estuarine conditions including aging(in air,in water),seawater anions(Cl^(-),Br^(-)and HCO_(3)^(-))and light on the HO^(·)production by pyrite *** one-electron transfer dominated the process from O_(2) to HO^(·)induced by oxidation of *** Fe(oxyhydr)oxide coatings on the surface of pyrite aged in air and water consumed hydrogen peroxide while mediating the electron transfer,and the combined effect of the two resulted in a suppression of HO^(·)production in the early stage of aging and a promotion of HO^(·)production in the later stage of *** of the surface oxide layers by aggressive anions was the main reason for the inhibition of HO^(·)production by Cl^(-)and Br^(-),and the generation of Cl^(·)and Br^(·)may also play a role in the scavenging of HO^(·).HCO_(3)^(-)increased the average rate of HO^(·)production through surface-CO_(2) complexes formed by adsorption on the surface of *** significant enhancement of HO^(·)production under light was attributed to the formation of photoelectrons induced by photochemical reactions on pyrite and its surface oxide *** findings provide new insights into the environmental chemical behavior of pyrite in the estuary and enrich the understanding of natural remediation of estuarine environments.

关键词： Hydroxyl radical Pyrite oxidation Aging Anions Irradiation

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Energy-absorbing porous materials:Bioinspired architecture and fabrication

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Nano Research 2024年第2期17卷 679-690页

作者： Junheng Zhao Meng Li Jiewei Chen Weiwei Gao Hao Bai State Key Laboratory of chemical engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China Department of Polymer Science and engineering Zhejiang UniversityHangzhou 310058China

Energy-absorbing materials are widely used in transportations,sports,and the military ***,porous materials,including natural and artificial materials,have attracted tremendous attentions due to their light weight and excellent energy absorption *** review summarizes the recent progresses in the natural and artificial energy-absorbing porous ***,we review the typical natural porous materials including cuttlebone,bighorn sheep horn,pomelo peel,and sunflower stem *** architectures,energy absorption abilities,and mechanisms of these typical natural materials and their bioinspired materials are ***,we provide a review on the fabrication methods of artificial energy-absorbing porous materials,such as conventional foaming and three-dimensional(3D)***,we address the challenges and prospects for the future development of energy-absorbing porous *** importantly,our review provides a direct guidance for the design and fabrication of energy-absorbing porous materials required for various engineering applications.

关键词： energy-absorbing porous materials natural materials natural structures bioinspired materials

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Vanadium(V) Complexes Containing Unsymmetrical N-Heterocyclic Carbene Ligands: Highly Efficient Synthesis and Catalytic Behavior towards Ethylene/Propylene Copolymerization

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Chinese Journal of Polymer Science 2024年第1期42卷 32-41,I0006页

作者： Yi-Cong Wang Hui Zhat Pei-Yi Cheng Shu Zhang Xiang-Wei Liu Yi-Xian Wu State Key Laboratory of chemical Resource engineering Beijing University of Chemical TechnologyBejing 100029China

The highly efficient method has been developed for the synthesis of NHC·VOCl_(3) containing symmetrical or unsymmetrical Nheterocyclic carbene(NHC) ligands by the transmetallation reaction of NHC·AgCl with VOCl_(3).The total isolated yield of VOCl_(3)[1,3-(2,4,6-Me_(3)C_(6)H_(2))_(2)(NCH=)_(2)C:](V4') reached 86% by transmetallation reaction,which is much higher than that(48%) by direct coordination *** methodology has also been used to synthesize the novel vanadium complexes containing unsymmetrical NHC ligands of VOCl_(3)[PhCH_(2)NCH=CHNR)C:](V5',R=2,4,6-Me_(3)C_(6)H_(2);V6',R=2,4-Me_(2)-6-Ph-C_(6)H_(2);V7',R=2,6-^(i)Pr_(2)-C_(6)H_(3)) with high yield,which could not be obtained by direct coordination *** catalytic activity and copolymerization ability would be improved by introducing unsymmetrical NHC ligands due to their less steric bulky *** vanadium complex V5' containing unsymmetrical NHC ligand exhibits higher catalytic activity(3.7×10^(5)g_(copolymer)·mol^(-1) of V·h^(-1)) than that of V4' containing symmetrical NHC ***,the higher propylene incorporation ratio(45.6 mol%) in the copolymers of ethylene with propylene could be obtained by using V5' than that(39.9%) by using V4'.The results would provide a highly efficient strategy for the synthesis of early transition metal complexes containing versitile NHC ligands,affording the catalyst with both high catalytic activity and copolymerization ability for the synthesis of high performance polyolefin elastomers.

关键词： Vanadium complex N-heterocyclic carbene ligand Transmetallation reaction Copolymerization of ethylene with propylene

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Synergistic enhancement of Ce-ZnO/g-C_(3)N_(4)photocatalytic performance using N,O-bis-vacancy induction and S-scheme heterojunctions

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Journal of Rare Earths 2024年第5期42卷 817-826,I0001页

作者： Guyu Zhang Yuan Zhang Xinlei Zhao Yujiang Jiao Yumin Yan Jianhui Jiang engineering Laboratory of chemical Resources Utilization in South Xinjiang of Xinjiang Production and Construction Corps College of Chemistry a Chemical EngineeringTarimUniversityAlar843300China

The photocatalytic decontamination of organic pollutants is an environmentally friendly and efficient water treatment *** introduction of vacancies,heterojunctions,and doping can enhance the performance of photocatalysts for such *** this study,N,O double-vacancy Ce-ZnO/g-C_(3)N_(4)S-scheme heterojunction photocatalysts were prepared,It is found that the electron separation and transfer efficiencies are considerably improved by the presence of nitrogen vacancies in graphitic ca rbon nitride(g-C_(3)N_(4))and oxygen vacancies in ZnO,in addition to the S-scheme heterojunction created between the two *** the degradation of methylene blue and ciprofloxacin,the degradation rates exhibited by Ce-ZnO/g-C_(3)N_(4)are significantly higher than those of the g=C_(3)N_(4)/ZnO *** remarkable photocatalytic performance of Ce-ZnO/g-C_(3)N_(4)may result from three key factors;(ⅰ)Ce doping,which produces impurity energy levels;(ⅱ)the generation of electron capture centres by the N and O vacancies;and(ⅲ)the synergistic effect of the S-type heterojunction formed at the interface between the two materials,This study therefore provides new approaches for the use of doping,vacancies,and heterojunctions to induce the efficient degradation of organic pollutants.

关键词： Photocatalysis Vacancy S-scheme Ce-ZnO/g-C_(3)N_(4) Degradation Rare earths

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Triple signal amplification electrochemical sensing platform for Hg^(2+) in water without direct modification of the working electrode

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Frontiers of environmental Science & engineering 2024年第7期18卷 157-167页

作者： Liuyin Hu Jiahua Cui Tao Lu Yalin Wang Jinping Jia School of environmental Science and engineering Shanghai Jiao Tong UniversityShanghai 200240China School of Chemistry and chemical engineering Shanghai Jiao Tong UniversityShanghai 200240China International Copper Association Ltd.Shanghai 200020China

An ultrasensitive electrochemical biosensor to detect trace Hg^(2+)in environmental samples was developed utilizing nanogold-decorated magnetic reduced graphene oxide(MrGO-AuNPs),exonuclease III-assisted target cycle(Exo Ⅲ-ATC)and hybridization chain reaction(HCR)synergistic triple signal *** MrGO-AuNPs is a superior carrier for capture DNA(cDNA)and acts as magnetic media for automatic separation and *** innovative utilization of the magnetism and improved sensing efficiency obviates the need for direct modification and repeated polishing of the working ***,the three DNA hairpins(cDNA,methylene blue(MB)labeled HP1 and HP2)further contribute to biosensor specificity and *** cDNA captures Hgt,it activates Exo Ⅲ-ATC due to the formation of a sticky end in the DNA stem via thymine-Hig-thymidine(T-Hg^(2+)-T),this leads to the hydrolysis of self-folded DNA by Exo Ⅲ-ATC to form"key"DNA(kDNA).The kDNA subsequently initiates HCR,resulting in massive super-sandwich structures(kDNA-[HP1/HP2])carrying signaling molecules on MrGO-AuNPs,and this overall structure serves as a signal probe(SP).Leveraging magnetic adsorption,the SP was automatically adsorbed onto the magneto-glass carbon electrode(MGCE),generating an amplified *** biosensor's detection limit(LOD)was 3.14 pmol/L,far below the limit of 10 nmol/L for mercury in drinking water set by the US *** biosensor also showed excellent selectivity when challenged by interfering ions,and the results of its application in actual samples indicate that it has good potential for practical applications in environmental monitoring.

关键词： Electrochemical sensing Hg^(2+) Amplification Graphene Hybridization chain reaction Exonuclease Ⅲ

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Sourcing the merits of 3D integrated air cathodes for highperformance Zn-air batteries by bubble pump consumption chronoamperometry

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Nano Research 2024年第8期17卷 6951-6959页

作者： Mengxuan Li Linfeng Yu Hai Liu Chuanyi Zhang Jiazhan Li Liang Luo Xiaoming Sun State Key Laboratory of chemical Resource engineering Beijing University of Chemical TechnologyBeijing 100029China

Zn-air batteries(ZABs)as a potential energy conversion system suffer from low power density(typically≤200 mW·cm^(−2)).Recently,three-dimensional(3D)integrated air cathodes have demonstrated promising performance over traditional twodimensional(2D)plane ones,which is ascribed to enriched active sites and enhanced diffusion,but without experimental ***,we applied a bubble pump consumption chronoamperometry(BPCC)method to quantitatively identify the gas diffusion coefficient(D)and effective catalytic sites density(ρEC)of the integrated air cathodes for ***,the D andρEC values can instruct consequent optimization on the growth of Co embedded N-doped carbon nanotubes(CoNCNTs)on carbon fiber paper(CFP)and aerophilicity tuning,giving 4 times D and 1.3 timesρEC over the conventional 2D Pt/C-CFP *** a result,using the CoNCNTs with half-wave potential of merely 0.78 V ***(Pt/C:0.89 V ***),the superaerophilic CoNCNTs-CFP cathode-based ZABs exhibited a superior peak power density of 245 mW·cm^(−2) over traditional 2D Pt/C-CFP counterparts,breaking the threshold of 200 mW·cm^(−2).This work reveals the intrinsic feature of the 3D integrated air cathodes by yielding exact D andρEC values,and demonstrates the feasibility of BPCC method for the optimization of integrated electrodes,bypassing trial-and-error strategy.

关键词： Zn-air batteries three-dimensional(3D)integrated air cathodes superaerophilic gas diffusion coefficient effective catalytic sites density

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Synthesis and modification of nanowires anchored on electrodes for electrochemical and electrophysical applications

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Nano Research 2024年第10期17卷 8863-8884页

作者： Feiyang Mo Zhitao Chen Nian Liu Xing Xie School of Civil and environmental engineering Georgia Institute of Technology311 Ferst Drive NWAtlantaGA 30332USA School of chemical and Biomolecular engineering Georgia Institute of Technology311 Ferst Drive NWAtlantaGA 30332USA

The integration of nanowires onto electrode surfaces marks a significant advancement over traditional electrode materials,conferring upon nanowire-modified electrodes a vast array of applications within electrochemical and electrophysical *** nanowires used for electrode modification can be catalogized into two distinct types:anchored nanowires and free-standing nanowires.A critical advantage of anchored nanowires lies in their enhanced electrical connectivity with the substrate,which reduces electrode resistance and facilitates charge ***,the anchorage of nanowires onto electrodes provides additional mechanical support,bolstering the structural stability of the nanowire ***,we review the development of anchored nanowires designed for applications in energy storage,electrocatalysis,and electric field treatment(EFT)over the past *** focus on the synthesis and modification strategies employed for anchored nanowires,culminating in the evaluation of these fabrication and enhancement *** this analysis,we aim to furnish comprehensive insights into the preparation of anchored nanowires,guiding the selection of appropriate fabrication processes and subsequent functional modifications.

关键词： electrode modification direct growth etching energy storage electrocatalysis electric field treatment

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