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Bridging molecular photosensitizer and Catalyst on carbon nanotubes toward enhanced selectivity and durability for CO_(2)photoreduction

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Journal of Environmental Sciences 2024年第6期140卷 157-164页

作者： Xiaofeng Cui Xueting Wang Lijun Zhao Jixin Wang Tingting Kong Yujie Xiong Anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China School of Chemistry and Chemical Engineering Anqing Normal UniversityAnqing 246011China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Homogenous molecular photoCatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-Catalyst assemblages,have been attracting extensive research interests due to their efficiency and customizability.However,their low durability and recyclability limit practical applications.In this work,we immobilized the Catalysts of metal terpyridyl complexes and the photosensitizer of[Ru(bpy)3]Cl2onto the surface of carbon nanotubes through covalent bonds and electrostatic interactions,respectively,transforming the homogeneous system into a heterogeneous one.Our characterizations prove that these metal complexes are well dispersed on CNTs with a high loading(ca.12 wt.%).Photocatalytic measurements reveal that catalytic activity is remarkably enhanced when the molecular Catalysts are anchored,which is three times higher than that of homogeneous molecular Catalysts.Moreover,when the photosensitizer of[Ru(bpy)3]Cl2is immobilized,the side reaction of hydrogen evolution is completely suppressed and the selectivity for CO production reaches 100%,with its durability also significantly improved.This work provides an effective pathway for constructing heterogeneous photoCatalysts based on rational assembly of efficient molecular photosensitizers and Catalysts.

关键词： durability selectivity Catalyst

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Facile molybdenum and aluminum recovery from spent hydrogenation Catalyst

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Chinese Journal of Chemical Engineering 2024年第5期69卷 72-78页

作者： Zhenhui Lv Jianan Li Dong Xue Tao Yang Gang Wang Chong Peng State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian 116024China Dalian Research Institute of Petroleum and Petrochemicals SINOPECDalian 116041China

Industrial Catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods.In this study,we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al_(2)O_(3) hydrogenation Catalysts through crystallization separation and coprecipitation.Furthermore,the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new Catalysts.Their properties were thoroughly analyzed and investigated using various characterization techniques.The hydrogenation activity of these newly prepared Catalysts was evaluated on a fixed-bed small-scale device and compared with a reference Catalyst synthesized from commercial raw reagents.Finally,the hydrogenation activity of the Catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil,specifically focusing on denitrogenation and aromatic saturation.This work not only offers an effective solution for recycling Catalysts but also promotes sustainable development.

关键词： Waste treatment Alumina Hydrogenation Catalyst Crystallization Precipitation

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Non-thermal atmospheric-pressure positive pulsating corona discharge in degradation of textile dye Reactive Blue 19 enhanced by Bi_(2)O_(3) Catalyst

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Plasma Science and Technology 2024年第2期26卷 104-113页

作者： Milica PETROVIC Dragan RADIVOJEVIC Sasa RANCEV Nena VELINOV Milos KOSTIC Danijela BOJIC Aleksandar BOJIC Department of Chemistry Faculty of Sciences and MathematicsUniversity of NisNis 18000Serbia Department of Physics Faculty of Sciences and MathematicsUniversity of NisNis 18000Serbia

In this work,monoclinic Bi_(2)O_(3) was applied for the first time,to the best of our knowledge,as a Catalyst in the process of dye degradation by a non-thermal atmospheric-pressure positive pulsating corona discharge.The research focused on the interaction of the plasma-generated species and the Catalyst,as well as the role of the Catalyst in the degradation process.Plasma decomposition of the anthraquinone reactive dye Reactive Blue 19(RB 19) was performed in a selfmade reactor system.Bi_(2)O_(3) was prepared by electrodeposition followed by thermal treatment,and characterized by x-ray diffraction,scanning electron microscopy and energy-dispersive xray techniques.It was observed that the Catalyst promoted decomposition of plasma-generated H_(2)O_(2) into ·OH radicals,the principal dye-degrading reagent,which further attacked the dye molecules.The Catalyst improved the decolorization rate by 2.5 times,the energy yield by 93.4%and total organic carbon removal by 7.1%.Excitation of the Catalyst mostly occurred through strikes by plasma-generated reactive ions and radical species from the air,accelerated by the electric field,as well as by fast electrons with an energy of up to 15 eV generated by the streamers reaching the liquid surface.These strikes transferred the energy to the Catalyst and created the electrons and holes,which further reacted with H_(2)O_(2) and water,producing ·OH radicals.This was indentified as the primary role of the Catalyst in this process.Decolorization reactions followed pseudo first-order kinetics.Production of H_(2)O_(2) and the dye degradation rate increased with increase in the input voltage.The optimal Catalyst dose was 500 mg·dm^(-3).The decolorization rate was a little lower in river water compared with that in deionized water due to the side reactions of ·OH radicals with organic matter and inorganic ions dissolved in the river water.

关键词： corona RB 19 Bi_(2)O_(3) Catalyst degradation

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Nitrogen–sulfur co-doped porous carbon derived from asphalt as efficient Catalyst for oxygen reduction

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Rare Metals 2024年第1期43卷 380-388页

作者： Jing-Sheng Ma Ming-Zai Wu Ling Chen Li-Xing Zhang Ying Xiong Key Laboratory of Structure and Functional Regulation of Hybrid Materials Ministry of EducationInstitute of EnergyHefei Comprehensive National Science CenterAnhui UniversityHefei 230601China

As an environment-friendly and low-cost petrochemical by-product, asphalt has great potential in the preparation of metal-free oxygen reduction electroCatalysts with excellent performance and outstanding stability. In this paper, we converted asphalt into porous carbon nanosheets by a simple activation method, using potassium citrate as the swelling agent.

关键词： stability porous Catalyst

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Improvement in hydrogen storage performance of MgH2 by vanadium doped with ZIF-8 derived a single-atom Catalyst V-N-C

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Rare Metals 2024年第6期43卷 2623-2635页

作者： Fei-Fan Hong Wei-Tao Shi Ruo-Lin Zhao Yi Fan Zi-Qi Liu Si-Zhi Ding Hai-Zhen Liu Wen-Zheng Zhou Jin Guo Zhi-Qiang Lan Guangxi Novel Battery Materials Research Center of Engineering Technology and Center on Nanoenergy Research Guangxi Colleges and Universities Key Laboratory of Blue Energy and Systems IntegrationCarbon Peak and Neutrality Science and Technology Development InstituteSchool of Physical Science and TechnologyGuangxi University Nanning Engineering Technology Research Center for Power Transmission System of New Energy Vehicle Transportation CollegeNanning University

Herein,the successful preparation of a singleatom Catalyst V-N-C using vanadium-doped zeolitic imidazolate framework（ZIF）-8 as a precursor is reported.The experimental results showed that the V-N-C had a good promoting effect on the hydrogen storage performance of MgH2,and the optimal addition amount of V-N-C was 10wt%.The hydrogenation and dehydrogenation apparent activation energies of 10 wt% V-N-C-catalyzed MgH2were reduced by 44.9 and 53.5 kJ·mol-1,respectively,compared to those of additive-free MgH2.The 10 wt% V-N-C-catalyzed MgH2could reabsorb 5.92 wt% of hydrogen in 50 min at 150℃,with a capacity retention rate of 99.1% after 30 cycles of hydrogen absorption and desorption.Mechanism analysis showed that V-N-C was partially transformed into VN and metallic V when it was milled with MgH2;the in-situ-formed VN and metallic V played an important role in improving the hydrogen storage performance of MgH2.This approach provides a potential solution for obtaining high-performance Mg-based hydrogen storage materials through synergistic interactions between V,N and C.

关键词： MgH 2 Hydrogen storage materials Catalyst Hydrogen storage perormance

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2D Ca/Nb-based perovskite oxide with Ta doping as highly efficient H_(2)O_(2)synthesis Catalyst

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Nano Research 2024年第6期17卷 4934-4942页

作者： Xingchen Yang Yang Gao Xiaohui Xu Wenqiang Xu Denghui Wang Bin Luo Dong Liu Tao Liang Bin Wang CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnologythe University of QueenslandSt LuciaQLD 4072Australia State Key Laboratory of Organic–Inorganic Composites College of Chemical EngineeringCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Hangzhou Institute for Advanced Study University of Chinese Academy of SciencesHangzhou 310024China State Key Lab of Silicon Materials Zhejiang UniversityHangzhou 310027China

Perovskite oxides(POs)are emerging as a class of highly efficient Catalysts for reducing oxygen to H_(2)O.Although a rich variety of POs-based Catalysts have been developed by tuning the complex composition,a highly efficient PO Catalyst that is able to alter the reaction pathway from a 4e−process to a 2e−process for H_(2)O_(2)production has rarely been achieved.We modified the structure and composition of a Ca-and Nb-based PO material by realizing a uniform two-dimensional(2D)morphology and varied Ta doping,resulting in the 2D Ca_(2)Nb_(3−x)Ta_(x)O_(10)−(x=0,0.5,1,and 1.5)monolayer Catalysts.The obtained Catalysts exhibit a dominant 2e−pathway and show exceptional H_(2)O_(2)production efficiency.The typical Ca_(2)Nb_(2.5)Ta_(0.5)O_(10)−nanoflakes showed an onset potential of 0.735 V vs.reversible hydrogen electrode(RHE),a remarkably high selectivity over 95%across a wide range of 0.3-0.7 V,an impressively high Faradaic efficiency of 94%,and a notable H_(2)O_(2)productivity of 1571 mmol·gcat^(−1)·h^(−1).These findings highlight the great potential of 2D perovskite oxide nanoflakes as advanced electroCatalysts for 2e−oxygen reduction reaction.

关键词： perovskite oxide H_(2)O_(2) two-electron oxygen reduction reaction Catalyst Ca_(2)Nb_(3-x)Ta_(x)O_(10)-nanoflakes

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Catalytic recycling of polyesters via a binuclear Catalyst

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Science China Chemistry 2024年第2期67卷 426-427页

作者： Bo Sun Ding Ma Beijing National Laboratory for Molecular Science New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

Plastics play a crucial role in modern society life. While the increasing use of plastics and rapid accumulation of plastic waste in nature environment have caused severe environmental crisis and the waste of carbon resources. Catalytic upcycling is a promising approach to transform plastic waste into high value-added chemicals to achieve a sustainable circular economy.

关键词： Catalytic polyester Catalyst

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Improved hydrogen storage kinetics of MgH_(2) using TiFe_(0.92)Mn_(0.04)Co_(0.04) with in-situ generated α-Fe as Catalyst

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Materials Reports(Energy) 2024年第1期4卷 95-103页

作者： Zefeng Li Yangfan Lu Jingfeng Wang Yu'an Chen Qian Li Fushen Pan College of Materials Science and Engineering National Engineering Research Center for Magnesium AlloysChongqing UniversityChongqing400044PR China National Key Laboratory of Advanced Casting Technologies Chongqing UniversityChongqing400044PR China Chongqing Institute of New Energy Storage Materials and Equipment Chongqing401135PR China

While TiFe alloy has recently attracted attention as the efficient Catalyst to enhance de/hydrogenation rates of Mg/MgH_(2),the difficulty of its activation characteristics has hindered further improvement of reaction kinetics.Herein,we report that the TiFe_(0.92)Mn_(0.04)Co_(0.04) Catalyst can overcome the abovementioned challenges.The synthesized MgH_(2)-30 wt% TiFe_(0.92)Mn_(0.04)Co_(0.04) can release 4.5 wt%of hydrogen in 16 min at 250℃,three times as fast as MgH_(2).The activation energy of dehydrogenation was as low as 84.6 kJ mol^(-1),which is 46.8%reduced from pure MgH_(2).No clear degradation of reaction rates and hydrogen storage capacity was observed for at least 30 cycles.Structural studies reveal that TiFe_(0.92)Mn_(0.04)Co_(0.04) partially decomposes to in-situ generatedα-Fe particles dispersed on TiFe_(0.92)Mn_(0.04)Co_(0.04).The presence ofα-Fe reduces the formation of an oxide layer on TiFe_(0.92)Mn_(0.04)Co_(0.04),enabling the activation processes.At the same time,the hydrogen incorporation capabilities of TiFe_(0.92)Mn_(0.04)Co_(0.04) can provide more hydrogen diffusion paths,which promote hydrogen dissociation and diffusion.These discoveries demonstrate the advanced nature and importance of combining the in-situ generatedα-Fe with TiFe_(0.92)Mn_(0.04)Co_(0.04).It provides a new strategy for designing highly efficient and stable Catalysts for Mg-based hydrogen storage materials.

关键词： Hydrogen storage materials Magnesium De/hydrogenation kinetics Catalyst

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Synergistic oxidation-reforming of biomass for high quality syngas production based on a bifunctional Catalyst

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Green Carbon 2024年第1期2卷 118-123页

作者： Tao He Dan Zhang Wenqing Chen Zeng Liu Ruidong Zhao Jianqing Li Jingli Wu Zhiqi Wang Jinhu Wu CAS Key Laboratory of Biofuels Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China Shandong Energy Institute Qingdao 266101China Qingdao New Energy Shandong Laboratory Qingdao 266101China University of Chinese Academy of Sciences Beijing 100049China

Conventional O_(2)gasification for low-rank biomass/sludge conversion is prone to high CO_(2)concentrations in the syngas because of its high O content and low calorific value.This study establishes a synergistic oxidationreforming reaction route for the conversion of low-rank carbon-containing resources into high-quality syngas.The efficient oxidation-reforming reaction is based on the bifunctional Catalyst NiO-Fe_(2)O_(3)/Al_(2)O_(3),which includes Fe_(2)O_(3) oxidation sites and NiO reforming sites.Hydrogen temperature-programmed reduction,together with X-ray diffraction and X-ray photoelectron spectroscopy experiments,demonstrated that the two functional active sites have strong interactions with the support,leading to efficient cooperation between the oxidation reaction and reforming reaction with regards to both the reaction sequence and C/H/O element balance.Syngas produced from biomass/sludge based on oxidation-reforming reactions has an extremely low CO_(2)concentration of approximately 3%,and the valid gas(CO,H_(2))concentration exceeds 95%.The valid gas yield of walnut shell reached 1452.9 mL/g,the total gas yield was 1507.2 mL/g,and the H_(2)/CO ratio was 1.02,which are all very close to the theoretical maximum values of 1553.1 mL/g and 1.01,respectively,demonstrating that the inherent CO_(2)/H_(2)O along with CH4/tar species were efficiently converted to H_(2)and CO through oxidation-reforming reactions.During a 60-cycle test,NiO-Fe_(2)O_(3)/Al_(2)O_(3) exhibited good redox stability.

关键词： Biomass Syngas Oxidation-reforming Bifunctional Catalyst

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A Cultural Catalyst--Bulgarian Sinologist brings Chinese culture closer to Mexicans

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Beijing Review 2024年第17期67卷 42-43页

作者： Juan Carlos Aguilar 不详

At the National School of Languages,Linguistics and Translation(ENALLT)at the National Autonomous University of Mexico in the country's capital of Mexico City,Sinologist Radina Dimitrova is recognized by both students... 详细信息

关键词： closer culture Catalyst

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