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Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction

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Nano Research 2024年第6期17卷 4807-4814页

作者： Runze Chen Xiaoying Wang Jianfei Dang Songjie Yun Liqiang Wang Fangong Kong You-Nian Liu State Key Laboratory of Biobased material and Green Papermaking Qilu University of TechnologyJinan 250353China School of material science and engineering Zhengzhou UniversityZhengzhou 450001China School of chemical engineering Zhengzhou UniversityZhengzhou 450001China Hunan Provincial Key Laboratory of Micro&Nano materials Interface science College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Carbon-supported single-atom catalysts were found to suffer reversible deactivation in catalytic hydrogenation,but the mechanism is still ***,nitro compounds hydrogenation catalyzed by N-doped carbon-supported Co single atom(Co1/NC)was taken as a model to uncover the mechanism of the reversible deactivation ***1/NC exhibited moderate adsorption towards the substrate molecules(i.e.,nitro compounds or related intermediates),which could be strengthened by the confinement effect from the porous ***,substrate molecules tend to accumulate within the pore channel,especially micropores that host Co1,making it difficult for the reactants to access the active sites and finally leading to their *** situation could be even worse when the substrate molecules possess a large ***,the catalytic activity of Co1/NC could be restored via a simple thermal treatment,which could remove the adsorbates within the pore channel,hence releasing active sites that were originally inaccessible to reactants.

关键词： single-atom catalysts porous carbon support reversible deactivation mechanistic study hydrogenation reaction

Process design and intensification of multicomponent azeotropes special distillation separation via molecular simulation and system optimization

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Chinese Journal of chemical engineering 2024年第7期71卷 24-44页

作者： Chunliang Liu Jianhui Zhong Ranran Wei Jiuxu Ruan Kaicong Wang Zhaoyou Zhu Yinglong Wang Limei Zhong college of chemical engineering Qingdao University of Science and TechnologyQingdao 266042China

This work provides an overview of distillation processes,including process design for different distillation processes,selection of entrainers for special distillation processes,system integration and intensification of distillation processes,optimization of process parameters for distillation processes and recent research progress in dynamic control ***,the feasibility of using thermodynamic topological theories such as residual curve,phase equilibrium line and distillation boundary line to analyze different separation regions is discussed,and the rationality of distillation process design is discussed by using its ***,the application of molecular simulation methods such as molecular dynamics simulation and quantum chemical calculation in the screening of entrainer is discussed for the extractive distillation *** thermal coupling mechanism of different distillation processes is used to explore the process of different process ***,a mixed integer nonlinear optimization strategy for the distillation process based on different algorithms is ***,the improvement of dynamic control strategies for different distillation processes in recent years is *** work focuses on the application of process intensification and system optimization in the design of distillation process,and analyzes the challenges,prospects,and development trends of distillation technology in the separation of multicomponent azeotropes.

关键词： Azeotrope separation Process design Optimization algorithm Process integration Dynamic control Entrainer selection

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 TechnologyZhenjiang212003China School of Chemistry and chemical engineering Liaocheng UniversityLiaocheng252000China School of material science and engineering Jiangsu University of Science and TechnologyZhenjiang212003China School of Environmental science and engineering Nanjing Tech UniversityNanjing210009China

Photothermal material applied in environmental governance has attracted growing *** 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 ***,a unique photothermal nanosphere with SiO_(2)core and thin carbon layer and dual Co-Mn oxides shell was allowed to form by sequential heat treatment in the inert atmosphere(SiO_(2)@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 *** state of bimetallic species was studied including their physical distribution,chemical valence,and interplay by various ***,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 SiO_(2)nanospheres(~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 *** 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 *** reactions condition controls and anion interference studies were conducted to identify the adaptability of the optimal ***,the application of solar-driven interfacial water evaporation using optimal SiO_(2)@Co_3Mn_1/C-600 catalyst was explored,showing a high water evaporation rate of 1.48 kg·m^(-2)·h^(-1)and 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

Coupling N-doping and confined Co_(3)O_(4) on carbon nanotubes by polydopamine coating strategy for pleiotropic water purification

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Rare Metals 2024年第7期43卷 3146-3160页

作者： Wen-Long Tu Gang Wang Yue Zhang Hong-Yang Zhu Rong-Rong Du Hong-Yao Zhao Sheng Tang Zeng-Jing Guo Jun Yang Fu Yang Cheng-Zhang Zhu School of Environmental and chemical engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Chemistry and chemical engineering Liaocheng UniversityLiaocheng 252000China School of material science and engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Environmental science and engineering Nanjing Tech UniversityNanjing 211816China

The development of effective and sustainable solutions for pleiotropic water purification becomes urgent and *** Fenton-like catalysts for activation of peroxymonosulfate(PMS)to purify organic wastewater show great *** this work,by tuning metal loading with an in-situ polydopamine coating strategy,oxygen vacancy-enriched Co_(3)O_(4) loading on N-doped carbon nanotubes(CNTs)were constructed to enhance PMS activation efficiency for pollutants ***,the obtained modified CNTs afford a well-developed N-containing network structure,which is further endowed with abundant Co(Ⅱ)/Co(Ⅲ)redox cycles and significant metal-carbon *** particular,the surface N doping in CNTs might induce the oriented enrichment of pollutants around the catalyst,which reduces the migration distance and correspondingly improves the utilization of reactive oxidative *** electron transfer efficiency of the catalyst can be further improved by incorporating oxygen vacancy-enriched Co_(3)O_(4).The performance results show that the optimal NC/Co-1 could mineralize 20×10^(-6)of bisphenol A(BPA)by almost 98%in 8 min.A low reaction activation energy(26.05 kJ·mol^(-1))in BPA degradation was demonstrated by the NC/*** importantly,NC/Co-1 can inherit excellent degradation performance towards oxytetracycline,2,4-dichlorophenol,and tetracycline,showing wide practical *** addition,by virtue of the photothermal conversion property,NC/Co-1 achieves an additive function for interfacial solar water evaporation(1.84 kg·m^(-2)·h^(-1),112.51%),showing impressive potential for clean water recovery under complicated environmental pollution conditions.

关键词： Carbon nanotube Advanced oxidation process Co_(3)O_(4) Photothermal conversion Solar water evaporation

Advances in noble metal-modified g-C3N4 heterostructures toward enhanced photocatalytic redox ability

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International Journal of Minerals, Metallurgy and materials 2024年第11期31卷 2368-2389页

作者： Zhang, Xiao Yang, Ping Faculty of chemical engineering and Technology Cracow University of Technology Krakow Poland School of material science & engineering University of Jinan Jinan China

The photocatalytic activity of catalysts depends on the energy-harvesting ability and the separation or transport of photogenerated carriers. The light absorption capacity of graphitic carbon nitride (g-C3N4)-based composites can be enhanced by adjusting the surface plasmon resonance (SPR) of noble metal nanoparticles (e.g., Cu, Au, and Pd) in the entire visible region. Adjustments can be carried out by varying the nanocomponents of the materials. The SPR of noble metals can enhance the local electromagnetic field and improve interband transition, and resonant energy transfer occurs from plasmonic dipoles to electron–hole pairs via near-field electromagnetic interactions. Thus, noble metals have emerged as relevant nanocomponents for g-C3N4 used in CO2 photoreduction and water splitting. Herein, recent key advances in noble metals (either in single atom, cluster, or nanoparticle forms) and composite photocatalysts based on inorganic or organic nanocomponent-incorporated g-C3N4 nanosheets are systematically discussed, including the applications of these photocatalysts, which exhibit improved photoinduced charge mobility in CO2 photoconversion and H2 production. Issues related to the different types of multi-nanocomponent heterostructures (involving Schottky junctions, Z-/S-scheme heterostructures, noble metals, and additional semiconductor nanocomponents) and the adjustment of dimensionality of heterostructures (by incorporating noble metal nanoplates on g-C3N4 forming 2D/2D heterostructures) are explored. The current prospects and possible challenges of g-C3N4 composite photocatalysts incorporated with noble metals (e.g., Au, Pt, Pd, and Cu), particularly in water splitting, CO2 reduction, pollution degradation, and chemical conversion applications, are summarized.

关键词： g-C3N4 heterostructure noble metal photocatalysis H_(2)generation CO_(2)

Accelerating solar driven CO_(2) reduction via sulfur-doping boosted water dissociation and proton transfer

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Nano Research 2024年第3期17卷 1056-1065页

作者： Ke Yan Liang Chen Yangguang Hu Ting Wang Cong Chen Chao Gao Youju Huang Benxia Li School of Chemistry and chemical engineering Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang ProvinceZhejiang Sci-Tech UniversityHangzhou 310018China college of material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhou 311121China School of Chemistry and materials science University of Science and Technology of ChinaHefei 230026China

Exploring efficient photocatalysts for solar driven CO_(2) reduction with water(H_(2)O)as a proton donor is highly imperative but remains a great challenge because the synchronous enhancement of CO_(2) activation,H_(2)O dissociation and proton transfer is hardly achieved on a ***,the sluggish H_(2)O dissociation impedes the photocatalytic CO_(2) reduction reaction involving multiple proton–electron coupling transfer ***,a sulfur-doped BiOCl(S-BiOCl)photocatalyst with abundant oxygen vacancies(OV)is developed,which exhibits broadband-light harvesting across solar spectrum and distinct photothermal effect due to *** photocatalytic CO_(2) reduction with H_(2)O in a gas–solid system,the high CO yield of 49.76μmol·g_(cat)^(-1)·h^(-1) with 100%selectivity is achieved over the S-BiOCl catalyst under a simulated *** H_(2)O-assisted CO_(2) reduction reaction on S-BiOCl catalyst is triggered by photocatalysis and the photothermal heating further enhances the reaction *** kinetic isotope experiments indicate that the sluggish H_(2)O dissociation affects the whole photocatalytic CO_(2) reduction *** presence of oxygen vacancies promotes the adsorption and activation of H_(2)O and CO_(2),and the doped S sites play a crucial role in boosting H_(2)O dissociation and accelerating the dynamic migration of hydrogen *** a result,the ingenious integration of OV defects,S sites and photothermal effect in S-BiOCl catalyst conjointly contributes to the significant improvement in photocatalytic CO_(2) reduction performance.

关键词： BiOCl sulfur doping photocatalytic CO_(2)reduction H_(2)O activation proton feeding

Tetrathiafulvalene esters with high redox potentials and improved solubilities for non-aqueous redox flow battery applications

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Green Energy & Environment 2024年第5期9卷 899-908页

作者： Weikang Hu Jiaqi Xu Nanjie Chen Zongcai Deng Yuekun Lai Dongyang Chen college of materials science and engineering Fuzhou UniversityFuzhou350116China college of chemical engineering Fuzhou UniversityFuzhou350116China

The exploitation of high performance redox-active substances is critically important for the development of non-aqueous redoxﬂow ***,three tetrathiofulvalene(TTF)derivatives with different substitution groups,namely TTF diethyl ester(TTFDE),TTF tetramethyl ester(TTFTM),and TTF tetraethyl ester(TTFTE),are prepared and their energy storage properties are *** has been found that the redox potential and solubility of these TTF derivatives in conventional carbonate electrolytes increases with the number of ester *** battery with a catholyte of 0.2 mol L^(-1) of TTFTE delivers a speciﬁc capacity of more than 10 Ah L^(-1) at the current density of 0.5 C with two discharge voltage platforms locating at as high as 3.85 and 3.60 V ***/Liþ.Its capacity retention can be improved from 2.34 Ah L^(-1) to 3.60 Ah L^(-1) after 100 cycles by the use of an anion exchange membrane to block the crossover of TTF *** excellent cycling stability of the TIF esters is supported by their well-delocalized electrons,as revealed by the density function theory ***,the introduction of more and larger electron-withdrawing groups is a promising strategy to simultaneously increase the redox-potential and solubility of redox-active ma-terials for non-aqueous redoxﬂow batteries.

关键词： Non-aqueous redox flow batteries Tetrathiofulvarene Redox potential Solubility Substituent effect

Bimagnetic metal constructed core-shell structure of Fe@Co nanowires for multi-band microwave absorption

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Progress in Natural science:materials International 2024年第02期34卷 354-361页

作者： Ping-an Yang Rui Cai Haibo Ruan Nanqing Zhang Xin Huang Rui Li Yuxin Zhang Yi Lu Zhihao Zhou School of Automation Chongqing University of Posts and Telecommunications Chongqing Key Laboratory of materials Surface & Interface science Chongqing University of Arts and Sciences college of engineering and Technology Zunyi Normal College college of material science and engineering Chongqing University

Controlled fabrication of materials by surface modification techniques has been a hot research topic. In this paper,one-dimensional(1D) core-shell structure Fe@Co nanowires(NWs) were successfully prepared by anchoring 0-dimensional(0D) Co nanoparticles on 1D Fe NWs based on the in situ reduction method. The electromagnetic parameters of the specimens at a filler mass fraction of 25 wt% were tested and the microwave loss mechanism was deeply analyzed. Binary magnetic metals in a core-shell structure have excellent multi-band microwave absorption capability(S-band, X-band and Ku-band). This is due to the heterogeneous interface and magnetic coupling effects tuning the dielectric and magnetic loss. This study offers a workable plan for creating effective multi-band magnetic metal-based microwave absorbers.

关键词： Core-shell structure Interface Magnetic coupling Microwave absorption One-dimensional nanowires

Fe3O4/Fe/FeS Tri-Heterojunction Node Spawning N-Carbon Nanotube Scaffold Structure for High-Performance Sodium-Ion Battery

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Energy & Environmental materials 2024年第4期7卷 143-152页

作者： Yuan Liu Qing Lin Xiaocui Chen Xufeng Meng Baoxiu Hou Haiyan Liu Shuaihua Zhang Ningzhao Shang Zheng Wang Chaoyue Zhang Jianjun Song Xiaoxian Zhao Department of Chemistry College of Science Hebei Agricultural University college of Chemistry and chemical engineering Qingdao University college of Physics Qingdao University

The Fe-based anode of sodium-ion batteries attracts much attention due to the abundant source,low-cost,and high specific ***,the low electron and ion transfer rate,poor structural stability,and shuttle effect of NaS2intermediate restrain its further ***,the Fe3O4/Fe/FeS tri-heterojunction node spawned N-carbon nanotube scaffold structure（FHNCS） was designed using the modified MIL-88B（Fe） as a template followed by catalytic growth and sulfidation process.

关键词： anode core-shell heterojunction hollow structure sodium ion batteries