COconversion via photocatalysis is a potential solution to address global warming and energy shortage.Photocatalysis can directly utilize the inexhaustible sunlight as an energy source to catalyze the reduction of COt...COconversion via photocatalysis is a potential solution to address global warming and energy shortage.Photocatalysis can directly utilize the inexhaustible sunlight as an energy source to catalyze the reduction of COto useful solar fuels such as CO, CH, CHOH, and CHOH. Among studied formulations, Cubased photocatalysts are the most attractive for COconversion because the Cu-based photocatalysts are low-cost and abundance comparing noble metal-based catalysts. In this literature review, a comprehensive summary of recent progress on Cu-based photocatalysts for COconversion, which includes metallic copper, copper alloy nanoparticles(NPs), copper oxides, and copper sulfides photocatalysts, can be found. This review also included a detailed discussion on the correlations of morphology, structure, and performance for each type of Cu-based catalysts. The reaction mechanisms and possible pathways for productions of various solar fuels were analyzed, which provide insight into the nature of potential active sites for the catalysts. Finally, the current challenges and perspective future research directions were outlined, holding promise to advance Cu-based photocatalysts for COconversion with much-enhanced energy conversion efficiency and production rates.展开更多
A key problem in CO_2 conversion by thermal plasma is suppressing the inverse reactions,CO?+?O?→?CO_2 and CO?+?0.5O_2?→?CO_2, to simultaneously obtain high CO yield and energy efficiency. This can be done by quickly...A key problem in CO_2 conversion by thermal plasma is suppressing the inverse reactions,CO?+?O?→?CO_2 and CO?+?0.5O_2?→?CO_2, to simultaneously obtain high CO yield and energy efficiency. This can be done by quickly quenching the decomposed gas or rapidly taking away free oxygen from decomposed gas. In this paper, experiments of CO_2 conversion by thermal plasma with carbon as a reducing agent are presented. Carbon quickly devoured free oxygen in thermal plasma decomposed gas, and not only is the inverse reaction completely suppressed, but the discharge energy to form oxygen atoms, oxygen molecular, and thermal energy is also reused.A CO_2 conversion rate of 67%–94% and the corresponding electric energy efficiency of about 70% are achieved, both are much higher than that seen so far by other plasma implementations.展开更多
The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving c...The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.展开更多
Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar f...Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar fuels.A surface-modified Ag@Ru-P25 photocatalyst with H_(2)O_(2) treatment was designed in this study to convert CO_(2) and H_(2)O vapor into highly selective CH4.Ru doping followed by Ag nanoparticles(NPs)cocatalyst deposition on P25(TiO_(2))enhances visible light absorption and charge separation,whereas H_(2)O_(2) treatment modifies the surface of the photocatalyst with hydroxyl(–OH)groups and promotes CO_(2) adsorption.High-resonance transmission electron microscopy,X-ray photoelectron spectroscopy,X-ray absorption near-edge structure,and extended X-ray absorption fine structure techniques were used to analyze the surface and chemical composition of the photocatalyst,while thermogravimetric analysis,CO_(2) adsorption isotherm,and temperature programmed desorption study were performed to examine the significance of H_(2)O_(2) treatment in increasing CO_(2) reduction activity.The optimized Ag1.0@Ru1.0-P25 photocatalyst performed excellent CO_(2) reduction activity into CO,CH4,and C2H6 with a~95%selectivity of CH4,where the activity was~135 times higher than that of pristine TiO_(2)(P25).For the first time,this work explored the effect of H_(2)O_(2) treatment on the photocatalyst that dramatically increases CO_(2) reduction activity.展开更多
Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for ...Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for n euro regeneration in the adult mammalian central ne rvous system.Howeve r,many questions remain regarding how a terminally differentiated glial cell can transform into a delicate neuron that forms part of the intricate brain circuitry.In addition,concerns have recently been raised around the absence of astrocyte-to-neuron conversion in astrocytic lineage-tra cing mice.In this study,we employed repetitive two-photon imaging to continuously capture the in situ astrocyte-to-neuron conversion process following ecto pic expression of the neural transcription factor NeuroD1 in both prolife rating reactive astrocytes and lineage-tra ced astrocytes in the mouse cortex.Time-lapse imaging over several wee ks revealed the ste p-by-step transition from a typical astrocyte with numero us short,tapered branches to a typical neuro n with a few long neurites and dynamic growth cones that actively explored the local environment.In addition,these lineage-converting cells were able to migrate ra dially or to ngentially to relocate to suitable positions.Furthermore,two-photon Ca2+imaging and patch-clamp recordings confirmed that the newly generated neuro ns exhibited synchronous calcium signals,repetitive action potentials,and spontaneous synaptic responses,suggesting that they had made functional synaptic connections within local neural circuits.In conclusion,we directly visualized the step-by-step lineage conversion process from astrocytes to functional neurons in vivo and unambiguously demonstrated that adult mammalian brains are highly plastic with respect to their potential for neuro regeneration and neural circuit reconstruction.展开更多
Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of...Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.展开更多
Electronic nose(eNose) is a modern bioelectronic sensor for monitoring biological processes that convert CO_(2) into valueadded products, such as products formed during photosynthesis and microbial fermentation. eNose...Electronic nose(eNose) is a modern bioelectronic sensor for monitoring biological processes that convert CO_(2) into valueadded products, such as products formed during photosynthesis and microbial fermentation. eNose technology uses an array of sensors to detect and quantify gases, including CO_(2), in the air. This study briefly introduces the concept of eNose technology and potential applications thereof in monitoring CO_(2) conversion processes. It also provides background information on biological CO_(2) conversion processes. Furthermore, the working principles of eNose technology vis-à-vis gas detection are discussed along with its advantages and limitations versus traditional monitoring methods. This study also provides case studies that have used this technology for monitoring biological CO_(2) conversion processes. eNose-predicted measurements were observed to be completely aligned with biological parameters for R~2 values of 0.864, 0.808, 0.802, and 0.948. We test eNose technology in a variety of biological settings, such as algae farms or bioreactors, to determine its effectiveness in monitoring CO_(2) conversion processes. We also explore the potential benefits of employing this technology vis-à-vis monitoring biological CO_(2) conversion processes, such as increased reaction efficiency and reduced costs versus traditional monitoring methods. Moreover, future directions and challenges of using this technology in CO_(2) capture and conversion have been discussed. Overall, we believe this study would contribute to developing new and innovative methods for monitoring biological CO_(2) conversion processes and mitigating climate change.展开更多
Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially acces...Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar guest species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.展开更多
Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(...Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.展开更多
The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical industry.Herein,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into th...The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical industry.Herein,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids (ILs) as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third component.It can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H_(2)S to a,β-unsaturated carboxylate esters.Also,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were investigated.Furthermore,the proposed interaction mechanism of H_(2)S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical calculation.The approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically benign.High-efficiency reaction activity can still be maintained after ten cycles of the catalyst.Therefore,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and cost-effective.It is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H_(2)S utilization,which will guide its application on an industrial scale.展开更多
The photoreduction of CO_(2)into CH_(4)with simultaneous high activity and selectivity is a promising strategy to increase energy supply and alleviate global warming.However,the absence of the active sites that is res...The photoreduction of CO_(2)into CH_(4)with simultaneous high activity and selectivity is a promising strategy to increase energy supply and alleviate global warming.However,the absence of the active sites that is responsible for the adsorption and activation of CO_(2)and the generation of CO and H2via side reactions often lead to poor efficiency and low selectivity of the catalyst.Herein,Cu,Pd,and PdCu metal clusters cocatalyst-anchored defective TiO_(2)nanotubes(Cu/TiO_(2)-SBO,Pd/TiO_(2)-SBO,and Pd1Cu1/TiO_(2)-SBO)were designed via a simple solution impregnation reduction and applied for photocatalytic conversion of CO_(2)to CH_(4).The Pd1Cu1/TiO_(2)-SBO photocatalyst exhibits excellent catalytic performance among the other catalysts for photoreduction of CO_(2)into CH_(4).More interestingly,the product selectivity of CH_(4)reaches up to 100%with a rate of 25μmol g^(-1)h^(-1).In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)simulations indicate that the main reasons for the high selectivity of CH_(4)are attributed to the PdCu alloy and oxygen vacancies,which jointly enhance the photoinduced carrier separation and lower energy barriers of key intermediates.Moreover,due to the tunable d-band center of the Cu site in the PdCu alloy,the generated intermediates can be well prevented from poisoning and promoted to participate in further reactions.Hopefully,the current study will provide insight into the development of new,highly selective photocatalysts for the visible light-catalytic reduction of CO_(2)into CH_(4).展开更多
Photoelectrochemical(PEC)energy conversion has emerged as a promising and efficient approach to sustainable energy harvesting and storage.By utilizing semiconductor photoelectrodes,PEC devices can harness solar energy...Photoelectrochemical(PEC)energy conversion has emerged as a promising and efficient approach to sustainable energy harvesting and storage.By utilizing semiconductor photoelectrodes,PEC devices can harness solar energy and drive electrochemical reactions such as water splitting or carbon dioxide(CO_(2))reduction to generate clean fuels and value-added chemicals.However,PEC energy conversion faces several challenges such as high overpotential,sluggish reaction kinetics,charge carrier recombination,and stability issues,which limit its practical implementation.Recently,significant research has been conducted to improve the overall conversion efficiency of PEC devices.One particularly promising approach is the use of cocatalysts,which involves introducing specific cocatalysts onto the photoelectrode surface to promote charge separation,improve reaction kinetics,and reduce the overpotential,thereby enhancing the overall performance of PEC energy conversion.This review provides a comprehensive overview of the recent developments in the earth-abundant cocatalysts for PEC water splitting and CO_(2) reduction.The main earth-abundant catalysts for the PEC water splitting include transition-metal dichalcogenide(TMD)-based materials,metal phosphides/carbides,and metal oxides/hydroxides.Meanwhile,PEC-CO_(2)RR was divided into C_(1) and C_(2+)based on the final product since various products could be produced,focusing on diverse earth-abundant materials-based cocatalysts.In addition,we provide and highlight key advancements achieved in the very recent reports on novel PEC system design engineering with cocatalysts.Finally,the current problems associated with PEC systems are discussed along with a suggested direction to overcome these obstacles.展开更多
This work describes the use of TiO_(2)nanotubes-based electrodes(TNT)modified with Cu_(2)O nanostructures and gold nanoparticles for the photoelectroreduction of CO_(2)to produce value-added compounds.A thin layer of ...This work describes the use of TiO_(2)nanotubes-based electrodes(TNT)modified with Cu_(2)O nanostructures and gold nanoparticles for the photoelectroreduction of CO_(2)to produce value-added compounds.A thin layer of polydopamine was used as both an adherent agent and an electron transfer mediator,due to itsπ-conjugated electron system.The highest production yield was achieved using a TNT@PDA/Nc/Au40%electrode,with Faradaic efficiencies of 47.4%(110.5μM cm^(-2))and 27.8%(50.4μM cm^(-2))for methanol and methane,respectively.The performance of the photoelectrodes was shown to be Cu_(2)O facet-dependent,with cubic structures leading to greater conversion of CO_(2)to methanol(43%)and methane(27%),compared to the octahedral morphology,while a higher percentage of metallic gold on the nanostructured Cu_(2)O surface was mainly important for CH4production.Density functional theory(DFT)calculations supported these findings,attributing the superior photoelectrocatalytic performance of the TNT@PDA/Nc/Au40%electrode for CH4generation to the formation of an OCH3intermediate bonded to Au atoms.Studies using isotope-labeling and analysis by gas chromatograph-mass(GC-MS)demonstrated that13CO_(2)was the source for photoelectrocatalytic generation of13CH3OH and13CH313CH2OH.展开更多
Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,bu...Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,but seldom do they exhibit excellent selectivity toward formate.In this article,we demonstrate that a heterointerface catalyst ZnO/ZnSnO3 with nanosheet morphology shows enhanced selectivity with a maximum Faradaic efficiency(FE)of 86%at−0.9 V versus reversible hydrogen electrode and larger current density for the conversion of CO_(2) to formate than pristine ZnO and ZnSnO3.In particular,the FEs of the C1 products(CO+HCOO−)exceed 98%over the potential window.The experimental measurements combined with theoretical calculations revealed that the ZnO in ZnO/ZnSnO3 heterojunction delivers the valence electron depletion and accordingly optimizes Zn d-band center,which results in moderate Zn-O hybridization of HCOO*and weakened Zn-C hybridization of competing COOH*,thus greatly boosting the HCOOH generation.Our study highlights the importance of charge redistribution in catalysts on the selectivity of electrochemical CO_(2) reduction.展开更多
The increasing atmospheric carbon dioxide (CO_(2)) concentration has exposed a series of crises in the earth's ecological environment.How to effectively fix and convert carbon dioxide into products with added valu...The increasing atmospheric carbon dioxide (CO_(2)) concentration has exposed a series of crises in the earth's ecological environment.How to effectively fix and convert carbon dioxide into products with added value has attracted the attention of many researchers.Cell-free enzyme catalytic system coupled with electrical and light have been a promising attempt in the field of biological carbon fixation in recent years.In this review,the research progresses of photoenzyme catalysis,electroenzyme catalysis and photo-electroenzyme catalysis for converting carbon dioxide into chemical products in cell-free systems are systematically summarized.We focus on reviewing and comparing various coupling methods and principles of photoenzyme catalysis and electroenzyme catalysis in cell-free systems,especially the materials used in the construction of the coupling system,and analyze and point out the characteristics and possible problems of different coupling methods.Finally,we discuss the major challenges and prospects of coupling physical signals and cell-free enzymatic catalytic systems in the field of CO_(2) fixation,suggesting possible strategies to improve the carbon sequestration capacity of such systems.展开更多
Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders....Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders. However, a few recent studies have claimed that neural transcription factors cannot convert astrocytes into neurons, attributing the converted neurons to pre-existing neurons mis-expressing transgenes. In this study, we overexpressed three distinct neural transcription factors––NeuroD1, Ascl1, and Dlx2––in reactive astrocytes in mouse cortices subjected to stab injury, resulting in a series of significant changes in astrocyte properties. Initially, the three neural transcription factors were exclusively expressed in the nuclei of astrocytes. Over time, however, these astrocytes gradually adopted neuronal morphology, and the neural transcription factors was gradually observed in the nuclei of neuron-like cells instead of astrocytes. Furthermore,we noted that transcription factor-infected astrocytes showed a progressive decrease in the expression of astrocytic markers AQP4(astrocyte endfeet signal), CX43(gap junction signal), and S100β. Importantly, none of these changes could be attributed to transgene leakage into preexisting neurons. Therefore, our findings suggest that neural transcription factors such as NeuroD1, Ascl1, and Dlx2 can effectively convert reactive astrocytes into neurons in the adult mammalian brain.展开更多
By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2...By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2) into CO.Generally,NiFe_(2_)O_(4) oxygen carriers have demonstrated remarkable efficiency in chemical looping CO_(2) conversion.Nevertheless,the intricate process of atomic migration and evolution within the internal structure of bimetallic oxygen carriers during continuous high‐temperature redox cycling remains unclear.Consequently,the lack of a fundamental understanding of the complex ionic migration and oxygen transfer associated with energy conversion processes hampers the design of high‐performance oxygen carriers.Thus,in this study,we employed in situ characterization techniques and theoretical calculations to investigate the ion migration behavior and structural evolution in the bulk of NiFe_(2_)O_(4) oxygen carriers during H_(2) reduction and CO_(2)/lab air oxidation cycles.We discovered that during the H_(2) reduction step,lattice oxygen rapidly migrates to vacancy layers to replenish consumed active oxygen species,while Ni leaches from the material and migrates to the surface.During the CO_(2) splitting step,Ni migrates toward the core of the bimetallic oxygen carrier,forming Fe–Ni alloys.During the air oxidation step,Fe–Ni migrates outward,creating a hollow structure owing to the Kirkendall effect triggered by the swift transfer of lattice oxygen.The metal atom migration paths depend on the oxygen transfer rates.These discoveries highlight the significance of regulating the release–recovery rate of lattice oxygen to uphold the structures and reactivity of oxygen carriers.This work offers a comprehensive understanding of the oxidation/reduction‐driven atomic interdiffusion behavior of bimetallic oxygen carriers.展开更多
Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electroche...Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)COOH.As a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni SACs.More importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.展开更多
Sulfur doped anatase TiO2 nanoparticles (3 nm- 12 nm) were synthesized by the reaction of titanium tetrachloride, water and sulfuric acid with addition of 3 M NaOH at room temperature. The electro-optical and photoc...Sulfur doped anatase TiO2 nanoparticles (3 nm- 12 nm) were synthesized by the reaction of titanium tetrachloride, water and sulfuric acid with addition of 3 M NaOH at room temperature. The electro-optical and photocatalytic properties of the synthesized sulfur doped TiO2 nanoparticles were studied along with Degussa commercial TiO2 particles (24 nm). The results show that band gap of TiO2 particles decreases from 3.31 to 3.25 eV and for that of commercial TiO2 to 3.2 eV when the particle sizes increased from 3 nm to 12 nm with increase in sulfur doping. The results of the photocatalytic activity under UV and sun radiation show maximum phenol conversion at the particle size of 4 nm at 4.80% S-doping. Similar results are obtained using UV energy for both phenol conversion and conversion of CO2+H2O in which formation of methanol, ethanol and proponal is observed. Production of methanol is also achieved on samples with a particle size of 8 and 12 nm and sulfur doping of 4.80% and 5.26%. For TiO2 particle of 4 nm without S doping, the production of methanol, ethanol and proponal was lower as compared to the S-doped particles. This is attributed to the combined electronic effect and band gap change, S dopant, specific surface area and the light source used.展开更多
基金financial supports from the National 1000 Young Talents Program of Chinathe National Nature Science Foundation of China (21603078)+1 种基金the National Materials Genome Project (2016YFB0700600)financial support from Research and Education in eNergy, Environment and Water (RENEW)Institute at the University at Buffalo, SUNY
文摘COconversion via photocatalysis is a potential solution to address global warming and energy shortage.Photocatalysis can directly utilize the inexhaustible sunlight as an energy source to catalyze the reduction of COto useful solar fuels such as CO, CH, CHOH, and CHOH. Among studied formulations, Cubased photocatalysts are the most attractive for COconversion because the Cu-based photocatalysts are low-cost and abundance comparing noble metal-based catalysts. In this literature review, a comprehensive summary of recent progress on Cu-based photocatalysts for COconversion, which includes metallic copper, copper alloy nanoparticles(NPs), copper oxides, and copper sulfides photocatalysts, can be found. This review also included a detailed discussion on the correlations of morphology, structure, and performance for each type of Cu-based catalysts. The reaction mechanisms and possible pathways for productions of various solar fuels were analyzed, which provide insight into the nature of potential active sites for the catalysts. Finally, the current challenges and perspective future research directions were outlined, holding promise to advance Cu-based photocatalysts for COconversion with much-enhanced energy conversion efficiency and production rates.
基金the supports of National Natural Science Foundation of China (Nos. 11775155, 51561135013, 21603202)
文摘A key problem in CO_2 conversion by thermal plasma is suppressing the inverse reactions,CO?+?O?→?CO_2 and CO?+?0.5O_2?→?CO_2, to simultaneously obtain high CO yield and energy efficiency. This can be done by quickly quenching the decomposed gas or rapidly taking away free oxygen from decomposed gas. In this paper, experiments of CO_2 conversion by thermal plasma with carbon as a reducing agent are presented. Carbon quickly devoured free oxygen in thermal plasma decomposed gas, and not only is the inverse reaction completely suppressed, but the discharge energy to form oxygen atoms, oxygen molecular, and thermal energy is also reused.A CO_2 conversion rate of 67%–94% and the corresponding electric energy efficiency of about 70% are achieved, both are much higher than that seen so far by other plasma implementations.
基金financial support from the King Abdullah University of Science and Technology(KAUST).
文摘The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.
基金supported by the Ministry of Science and ICT in Korea(2021R1A2C2009459)X-ray absorption spectra were obtained from Pohang Accelerator Laboratory(PAL)10C beamlinesupported by the US Department of Energy,Office of Science,Office of Advanced Scientific Computing Research,and Scientific Discovery through Advanced Computing(SciDAC)program under Award Number DE-SC0022209.
文摘Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar fuels.A surface-modified Ag@Ru-P25 photocatalyst with H_(2)O_(2) treatment was designed in this study to convert CO_(2) and H_(2)O vapor into highly selective CH4.Ru doping followed by Ag nanoparticles(NPs)cocatalyst deposition on P25(TiO_(2))enhances visible light absorption and charge separation,whereas H_(2)O_(2) treatment modifies the surface of the photocatalyst with hydroxyl(–OH)groups and promotes CO_(2) adsorption.High-resonance transmission electron microscopy,X-ray photoelectron spectroscopy,X-ray absorption near-edge structure,and extended X-ray absorption fine structure techniques were used to analyze the surface and chemical composition of the photocatalyst,while thermogravimetric analysis,CO_(2) adsorption isotherm,and temperature programmed desorption study were performed to examine the significance of H_(2)O_(2) treatment in increasing CO_(2) reduction activity.The optimized Ag1.0@Ru1.0-P25 photocatalyst performed excellent CO_(2) reduction activity into CO,CH4,and C2H6 with a~95%selectivity of CH4,where the activity was~135 times higher than that of pristine TiO_(2)(P25).For the first time,this work explored the effect of H_(2)O_(2) treatment on the photocatalyst that dramatically increases CO_(2) reduction activity.
基金supported by the National Natural Science Foundation of China,No.31970906(to WLei)the Natural Science Foundation of Guangdong Province,No.2020A1515011079(to WLei)+4 种基金Key Technologies R&D Program of Guangdong Province,No.2018B030332001(to GC)Science and Technology Projects of Guangzhou,No.202206060002(to GC)the Youth Science Program of the National Natural Science Foundation of China,No.32100793(to ZX)the Pearl River Innovation and Entrepreneurship Team,No.2021ZT09 Y552Yi-Liang Liu Endowment Fund from Jinan University Education Development Foundation。
文摘Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for n euro regeneration in the adult mammalian central ne rvous system.Howeve r,many questions remain regarding how a terminally differentiated glial cell can transform into a delicate neuron that forms part of the intricate brain circuitry.In addition,concerns have recently been raised around the absence of astrocyte-to-neuron conversion in astrocytic lineage-tra cing mice.In this study,we employed repetitive two-photon imaging to continuously capture the in situ astrocyte-to-neuron conversion process following ecto pic expression of the neural transcription factor NeuroD1 in both prolife rating reactive astrocytes and lineage-tra ced astrocytes in the mouse cortex.Time-lapse imaging over several wee ks revealed the ste p-by-step transition from a typical astrocyte with numero us short,tapered branches to a typical neuro n with a few long neurites and dynamic growth cones that actively explored the local environment.In addition,these lineage-converting cells were able to migrate ra dially or to ngentially to relocate to suitable positions.Furthermore,two-photon Ca2+imaging and patch-clamp recordings confirmed that the newly generated neuro ns exhibited synchronous calcium signals,repetitive action potentials,and spontaneous synaptic responses,suggesting that they had made functional synaptic connections within local neural circuits.In conclusion,we directly visualized the step-by-step lineage conversion process from astrocytes to functional neurons in vivo and unambiguously demonstrated that adult mammalian brains are highly plastic with respect to their potential for neuro regeneration and neural circuit reconstruction.
基金support from the Tangshan Talent Funding Project(Grant No.A202202007)National Natural Science Foundation of China(Grant Nos.22102136 and 21703065)+2 种基金Natural Science Foundation of Hebei Province(Grant Nos.B2018209267 and E2022209039)Natural Science Foundation of Hubei Province(Grant No.2022CFB1001)Department of Education of Hubei Province(Grant No.Q20221701).
文摘Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.
基金supported by the National Key Technologies R & D Program of China during the 14th Five-Year Plan period (No. 2021YFD1700904)Henan Provincial Important Project (No. 221100320200)+1 种基金State Key Laboratory of Wheat and Maize Crap Science (No. SKL2023ZZ09)the Henan Center for Outstanding Overseas Scientists (No. GZS2021007)。
文摘Electronic nose(eNose) is a modern bioelectronic sensor for monitoring biological processes that convert CO_(2) into valueadded products, such as products formed during photosynthesis and microbial fermentation. eNose technology uses an array of sensors to detect and quantify gases, including CO_(2), in the air. This study briefly introduces the concept of eNose technology and potential applications thereof in monitoring CO_(2) conversion processes. It also provides background information on biological CO_(2) conversion processes. Furthermore, the working principles of eNose technology vis-à-vis gas detection are discussed along with its advantages and limitations versus traditional monitoring methods. This study also provides case studies that have used this technology for monitoring biological CO_(2) conversion processes. eNose-predicted measurements were observed to be completely aligned with biological parameters for R~2 values of 0.864, 0.808, 0.802, and 0.948. We test eNose technology in a variety of biological settings, such as algae farms or bioreactors, to determine its effectiveness in monitoring CO_(2) conversion processes. We also explore the potential benefits of employing this technology vis-à-vis monitoring biological CO_(2) conversion processes, such as increased reaction efficiency and reduced costs versus traditional monitoring methods. Moreover, future directions and challenges of using this technology in CO_(2) capture and conversion have been discussed. Overall, we believe this study would contribute to developing new and innovative methods for monitoring biological CO_(2) conversion processes and mitigating climate change.
基金supported by the National Key R&D program of China(2019YFA0706802)National Natural Science Foundation of China(52063029)+2 种基金Natural Science Basic Research Program of Shaanxi(2022JM-200,2021JQ-716)China Postdoctoral Science Foundation(2020M672269)Doctoral Research Program of Yan’an University(YDBK2019-02)
文摘Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar guest species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.
基金supported by the National Key R&D Program of China(2022YFA2105900)the National Natural Science Foundation of China(No.22178197)。
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.
基金sponsored by the National Natural Science Foundation of China (Nos. 22208140 and 22078145)。
文摘The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical industry.Herein,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids (ILs) as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third component.It can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H_(2)S to a,β-unsaturated carboxylate esters.Also,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were investigated.Furthermore,the proposed interaction mechanism of H_(2)S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical calculation.The approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically benign.High-efficiency reaction activity can still be maintained after ten cycles of the catalyst.Therefore,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and cost-effective.It is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H_(2)S utilization,which will guide its application on an industrial scale.
基金the financial support from the Program for Innovative Research Team in University of Henan Province(21IRTSTHN009)Science and Technology Fund of Henan Province(225200810051)Natural Science Foundation of Henan Province(222300420406)。
文摘The photoreduction of CO_(2)into CH_(4)with simultaneous high activity and selectivity is a promising strategy to increase energy supply and alleviate global warming.However,the absence of the active sites that is responsible for the adsorption and activation of CO_(2)and the generation of CO and H2via side reactions often lead to poor efficiency and low selectivity of the catalyst.Herein,Cu,Pd,and PdCu metal clusters cocatalyst-anchored defective TiO_(2)nanotubes(Cu/TiO_(2)-SBO,Pd/TiO_(2)-SBO,and Pd1Cu1/TiO_(2)-SBO)were designed via a simple solution impregnation reduction and applied for photocatalytic conversion of CO_(2)to CH_(4).The Pd1Cu1/TiO_(2)-SBO photocatalyst exhibits excellent catalytic performance among the other catalysts for photoreduction of CO_(2)into CH_(4).More interestingly,the product selectivity of CH_(4)reaches up to 100%with a rate of 25μmol g^(-1)h^(-1).In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)simulations indicate that the main reasons for the high selectivity of CH_(4)are attributed to the PdCu alloy and oxygen vacancies,which jointly enhance the photoinduced carrier separation and lower energy barriers of key intermediates.Moreover,due to the tunable d-band center of the Cu site in the PdCu alloy,the generated intermediates can be well prevented from poisoning and promoted to participate in further reactions.Hopefully,the current study will provide insight into the development of new,highly selective photocatalysts for the visible light-catalytic reduction of CO_(2)into CH_(4).
基金supported by the National Research Foundation of Korea (NRF)funded by the Korean government (2021R1A4A3027878,2022M3H4A1A01012712)。
文摘Photoelectrochemical(PEC)energy conversion has emerged as a promising and efficient approach to sustainable energy harvesting and storage.By utilizing semiconductor photoelectrodes,PEC devices can harness solar energy and drive electrochemical reactions such as water splitting or carbon dioxide(CO_(2))reduction to generate clean fuels and value-added chemicals.However,PEC energy conversion faces several challenges such as high overpotential,sluggish reaction kinetics,charge carrier recombination,and stability issues,which limit its practical implementation.Recently,significant research has been conducted to improve the overall conversion efficiency of PEC devices.One particularly promising approach is the use of cocatalysts,which involves introducing specific cocatalysts onto the photoelectrode surface to promote charge separation,improve reaction kinetics,and reduce the overpotential,thereby enhancing the overall performance of PEC energy conversion.This review provides a comprehensive overview of the recent developments in the earth-abundant cocatalysts for PEC water splitting and CO_(2) reduction.The main earth-abundant catalysts for the PEC water splitting include transition-metal dichalcogenide(TMD)-based materials,metal phosphides/carbides,and metal oxides/hydroxides.Meanwhile,PEC-CO_(2)RR was divided into C_(1) and C_(2+)based on the final product since various products could be produced,focusing on diverse earth-abundant materials-based cocatalysts.In addition,we provide and highlight key advancements achieved in the very recent reports on novel PEC system design engineering with cocatalysts.Finally,the current problems associated with PEC systems are discussed along with a suggested direction to overcome these obstacles.
基金FAPESP,Brazil(#2023/10027-5,#2014/50945-4,#2020/15230-5,and#2021/000675-4)CNPq,Brazil(#465571/2014-0,#303269/2021-9,and#307837/2014-9)+6 种基金Instituto Serrapilheira(grant number Serra-2211-41925)FAPEMIG,Brazil(#PPM-00831-15)for support of this workCNPq,Brazil(#105944/2022-0)and PROPEUNESP(13/2022)FAPESP(#2019/00463-7,#2018/22845-6,and#2021/08007-0,respectively)for scholarshipsthe National Institute for Alternative Technologies of Detection,Toxicological Evaluation and Removal of Micropollutants and Radioactives(INCT-DATREM)the support of the Research Centre for Greenhouse Gas Innovation(RCGI),hosted by the University of Sao Paulo(USP)and sponsored by FAPESP and Shell Brasilthe strategic support given by ANP,Brazil(Brazilian National Oil,Natural Gas,and Biofuels Agency)through the R&D levy regulation。
文摘This work describes the use of TiO_(2)nanotubes-based electrodes(TNT)modified with Cu_(2)O nanostructures and gold nanoparticles for the photoelectroreduction of CO_(2)to produce value-added compounds.A thin layer of polydopamine was used as both an adherent agent and an electron transfer mediator,due to itsπ-conjugated electron system.The highest production yield was achieved using a TNT@PDA/Nc/Au40%electrode,with Faradaic efficiencies of 47.4%(110.5μM cm^(-2))and 27.8%(50.4μM cm^(-2))for methanol and methane,respectively.The performance of the photoelectrodes was shown to be Cu_(2)O facet-dependent,with cubic structures leading to greater conversion of CO_(2)to methanol(43%)and methane(27%),compared to the octahedral morphology,while a higher percentage of metallic gold on the nanostructured Cu_(2)O surface was mainly important for CH4production.Density functional theory(DFT)calculations supported these findings,attributing the superior photoelectrocatalytic performance of the TNT@PDA/Nc/Au40%electrode for CH4generation to the formation of an OCH3intermediate bonded to Au atoms.Studies using isotope-labeling and analysis by gas chromatograph-mass(GC-MS)demonstrated that13CO_(2)was the source for photoelectrocatalytic generation of13CH3OH and13CH313CH2OH.
基金National Natural Science Foundation of China,Grant/Award Number:22102079Taishan Scholar Program of Shandong Province,China,Grant/Award Number:tsqn202211162Natural Science Foundation of Shandong Province of China,Grant/Award Numbers:ZR2021YQ10,ZR2022QB163。
文摘Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,but seldom do they exhibit excellent selectivity toward formate.In this article,we demonstrate that a heterointerface catalyst ZnO/ZnSnO3 with nanosheet morphology shows enhanced selectivity with a maximum Faradaic efficiency(FE)of 86%at−0.9 V versus reversible hydrogen electrode and larger current density for the conversion of CO_(2) to formate than pristine ZnO and ZnSnO3.In particular,the FEs of the C1 products(CO+HCOO−)exceed 98%over the potential window.The experimental measurements combined with theoretical calculations revealed that the ZnO in ZnO/ZnSnO3 heterojunction delivers the valence electron depletion and accordingly optimizes Zn d-band center,which results in moderate Zn-O hybridization of HCOO*and weakened Zn-C hybridization of competing COOH*,thus greatly boosting the HCOOH generation.Our study highlights the importance of charge redistribution in catalysts on the selectivity of electrochemical CO_(2) reduction.
基金supported by the National Key R&D Program of China (2018YFA0901700)National Natural Science Foundation of China (22278241)+1 种基金a grant from the Institute Guo Qiang, Tsinghua University (2021GQG1016)Department of Chemical Engineering-iBHE Joint Cooperation Fund。
文摘The increasing atmospheric carbon dioxide (CO_(2)) concentration has exposed a series of crises in the earth's ecological environment.How to effectively fix and convert carbon dioxide into products with added value has attracted the attention of many researchers.Cell-free enzyme catalytic system coupled with electrical and light have been a promising attempt in the field of biological carbon fixation in recent years.In this review,the research progresses of photoenzyme catalysis,electroenzyme catalysis and photo-electroenzyme catalysis for converting carbon dioxide into chemical products in cell-free systems are systematically summarized.We focus on reviewing and comparing various coupling methods and principles of photoenzyme catalysis and electroenzyme catalysis in cell-free systems,especially the materials used in the construction of the coupling system,and analyze and point out the characteristics and possible problems of different coupling methods.Finally,we discuss the major challenges and prospects of coupling physical signals and cell-free enzymatic catalytic systems in the field of CO_(2) fixation,suggesting possible strategies to improve the carbon sequestration capacity of such systems.
基金supported by the Key Project of Guangzhou City,No.202206060002Science and Technology Project of Guangdong Province,No.2018B030332001Guangdong Provincial Pearl River Project,No.2021ZT09Y552 (all to GC)。
文摘Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders. However, a few recent studies have claimed that neural transcription factors cannot convert astrocytes into neurons, attributing the converted neurons to pre-existing neurons mis-expressing transgenes. In this study, we overexpressed three distinct neural transcription factors––NeuroD1, Ascl1, and Dlx2––in reactive astrocytes in mouse cortices subjected to stab injury, resulting in a series of significant changes in astrocyte properties. Initially, the three neural transcription factors were exclusively expressed in the nuclei of astrocytes. Over time, however, these astrocytes gradually adopted neuronal morphology, and the neural transcription factors was gradually observed in the nuclei of neuron-like cells instead of astrocytes. Furthermore,we noted that transcription factor-infected astrocytes showed a progressive decrease in the expression of astrocytic markers AQP4(astrocyte endfeet signal), CX43(gap junction signal), and S100β. Importantly, none of these changes could be attributed to transgene leakage into preexisting neurons. Therefore, our findings suggest that neural transcription factors such as NeuroD1, Ascl1, and Dlx2 can effectively convert reactive astrocytes into neurons in the adult mammalian brain.
基金National Natural Science Foundation of China,Grant/Award Numbers:52076209,52006224,52106285,22179027Foundation and Applied Foundation Research of Guangdong Province,Grant/Award Number:2022B1515020045+1 种基金Natural Science Foundation of Guangxi Province,Grant/Award Number:2021GXNSFAA075036Young Talent Support Project of Guangzhou Association for Science and Technology,Grant/Award Number:QT‐2023‐042。
文摘By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2) into CO.Generally,NiFe_(2_)O_(4) oxygen carriers have demonstrated remarkable efficiency in chemical looping CO_(2) conversion.Nevertheless,the intricate process of atomic migration and evolution within the internal structure of bimetallic oxygen carriers during continuous high‐temperature redox cycling remains unclear.Consequently,the lack of a fundamental understanding of the complex ionic migration and oxygen transfer associated with energy conversion processes hampers the design of high‐performance oxygen carriers.Thus,in this study,we employed in situ characterization techniques and theoretical calculations to investigate the ion migration behavior and structural evolution in the bulk of NiFe_(2_)O_(4) oxygen carriers during H_(2) reduction and CO_(2)/lab air oxidation cycles.We discovered that during the H_(2) reduction step,lattice oxygen rapidly migrates to vacancy layers to replenish consumed active oxygen species,while Ni leaches from the material and migrates to the surface.During the CO_(2) splitting step,Ni migrates toward the core of the bimetallic oxygen carrier,forming Fe–Ni alloys.During the air oxidation step,Fe–Ni migrates outward,creating a hollow structure owing to the Kirkendall effect triggered by the swift transfer of lattice oxygen.The metal atom migration paths depend on the oxygen transfer rates.These discoveries highlight the significance of regulating the release–recovery rate of lattice oxygen to uphold the structures and reactivity of oxygen carriers.This work offers a comprehensive understanding of the oxidation/reduction‐driven atomic interdiffusion behavior of bimetallic oxygen carriers.
基金financially supported by the Natural Science Foundation of Shandong Province (ZR2020QB132,ZR2020MB025)the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL202108SIC)the Taishan Scholar Program of Shandong Province (ts201712046)。
文摘Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)COOH.As a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni SACs.More importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.
文摘Sulfur doped anatase TiO2 nanoparticles (3 nm- 12 nm) were synthesized by the reaction of titanium tetrachloride, water and sulfuric acid with addition of 3 M NaOH at room temperature. The electro-optical and photocatalytic properties of the synthesized sulfur doped TiO2 nanoparticles were studied along with Degussa commercial TiO2 particles (24 nm). The results show that band gap of TiO2 particles decreases from 3.31 to 3.25 eV and for that of commercial TiO2 to 3.2 eV when the particle sizes increased from 3 nm to 12 nm with increase in sulfur doping. The results of the photocatalytic activity under UV and sun radiation show maximum phenol conversion at the particle size of 4 nm at 4.80% S-doping. Similar results are obtained using UV energy for both phenol conversion and conversion of CO2+H2O in which formation of methanol, ethanol and proponal is observed. Production of methanol is also achieved on samples with a particle size of 8 and 12 nm and sulfur doping of 4.80% and 5.26%. For TiO2 particle of 4 nm without S doping, the production of methanol, ethanol and proponal was lower as compared to the S-doped particles. This is attributed to the combined electronic effect and band gap change, S dopant, specific surface area and the light source used.