Ammonia is essential for agriculture and,as a next-generation carbon-free fuel,typically produced through the Haber-Bosch method.This process requires high temperature and pressure,leading to significant energy consum...Ammonia is essential for agriculture and,as a next-generation carbon-free fuel,typically produced through the Haber-Bosch method.This process requires high temperature and pressure,leading to significant energy consumption and greenhouse gas emissions.Therefore,achieving ammonia synthesis under milder conditions has been a long-standing goal.In this study,we design and synthesize a series of CeO_(2)-modified Fe/carbon-based catalysts with varying amounts of CeO_(2)(Ce_(x)Fe_(y)/C).The catalyst Ce_(2)Fe_(5)/C demonstrates an ammonia yield rate of 3.5 mmol/(g·h),which is 44 times greater than that of Fe/C and 8 times greater than that of commercial Fe-based catalysts at 300℃and 1 MPa.Temperature-programmed desorption experiments show that Ce_(2)Fe_(5)/C has enhanced nitrogen adsorption capabilities.Multiple analyses confirm that the CeO_(2)in Ce_(2)Fe_(5)/C is rich in oxygen vacancies,which can provide electrons to Fe,facilitating nitrogen adsorption,dissociation,and activity in low-temperature ammonia synthesis.展开更多
The development of human industry inevitably leads to excessive carbon dioxide(CO_(2))emissions.It can cause critical ecological consequences,primarily global warming and ocean acidification.In this regard,close atten...The development of human industry inevitably leads to excessive carbon dioxide(CO_(2))emissions.It can cause critical ecological consequences,primarily global warming and ocean acidification.In this regard,close attention is paid to the carbon capture,utilization,and storage concept.The key component of this concept is the catalytic conversion of CO_(2)into valuable chemical compounds and fuels.Light olefins are one of the most industrially important chemicals,and their sustainable production via CO_(2)hydrogenation could be a prospective way to reach carbon neutrality.Fe-based materials are widely recognized as effective thermocatalysts and photothermal catalysts for that process thanks to their low cost,high activity,and good stability.This review critically examines the most recent progress in the development and optimization of Fe-based catalysts for CO_(2)hydrogenation into light olefins.Particular attention is paid to understanding the roles of catalyst composition,structural properties,and promoters in enhancing catalytic activity,selectivity,and stability.展开更多
Regulating the location of the metal promoters plays a vital role in catalyst structure and its catalytic behavior during CO_(2)hydrogenation to higher alcohols.Herein,we selected the metal promoters with a precipitat...Regulating the location of the metal promoters plays a vital role in catalyst structure and its catalytic behavior during CO_(2)hydrogenation to higher alcohols.Herein,we selected the metal promoters with a precipitation pH similar to that of Cu^(2+)or Fe^(3+)to prepare a series of CuFe-based catalysts.Characterization results show that doping Al or Cr promoter,located with the Fe phase,suppressed the excessive carburization of the Fe phase and maintained an optimal proportion between Fe_(3)O_(4) and amorphous iron carbide(FeC_(x)),thus exhibiting superior catalytic activity and stability.In contrast,doping Zn or In promoter,located with the Cu phase,underwent a deeper carburization and formed more crys-talline FeC_(x),showing an inferior performance.The CuFeCr catalyst achieved the highest space-time yield of 330 mg g_(cat)^(-1)h^(-1)for higher alcohols among these catalysts.This study provides a novel strategy for opti-mizing the structure of the active phases for CO_(2)hydrogenation.展开更多
Fe‐based catalysts for the production of light olefins via the Fischer‐Tropsch synthesis were modi‐fied by adding a Zn promoter using both microwave‐hydrothermal and impregnation methods. The physicochemical prope...Fe‐based catalysts for the production of light olefins via the Fischer‐Tropsch synthesis were modi‐fied by adding a Zn promoter using both microwave‐hydrothermal and impregnation methods. The physicochemical properties of the resulting catalysts were determined by scanning electron mi‐croscopy, the Brunauer‐Emmett‐Teller method, X‐ray diffraction, H2 temperature‐programed re‐duction and X‐ray photoelectron spectroscopy. The results demonstrate that the addition of a Zn promoter improves both the light olefin selectivity over the catalyst and the catalyst stability. The catalysts prepared via the impregnation method, which contain greater quantities of surface ZnO, exhibit severe carbon deposition following activity trials. In contrast, those materials synthesized using the microwave‐hydrothermal approach show improved dispersion of Zn and Fe phases and decreased carbon deposition, and so exhibit better CO conversion and stability.展开更多
Metallurgical dust(MD)was used as raw material to prepare rare earth Ce-doped Fe-based catalysts.The results show that the Ce_(0.1)/AMD-300℃catalyst prepared from acid-modified diatomite(AMD)with mCe/mMD=0.1(m_(Ce)an...Metallurgical dust(MD)was used as raw material to prepare rare earth Ce-doped Fe-based catalysts.The results show that the Ce_(0.1)/AMD-300℃catalyst prepared from acid-modified diatomite(AMD)with mCe/mMD=0.1(m_(Ce)and m_(MD)are the mass of Ce and MD,respectively)after being roasted at 300℃can reach 99%NO_(x)removal rate in the wide temperature range of 230–430℃and exhibits excellent So_(2)and H_(2)o resistance.The MD effectively removes alkali metal elements by the modification process,increases the specific surface area and optimizes the pore structure of MD.The doping of Ce element makes Fe-based catalysts have more surface adsorbed oxygen O_(α)and a higher Ce^(3+)/Ce^(4+)ratio.Through ammonia temperature-programmed desorption and hydrogen temperature-programmed reduction,it was found that the strong interaction between cerium and iron promotes the formation of more oxygen cavities in the catalyst,thereby generating more active and easily reducible oxygen species and promoting the transformation of Brønsted acid site to Lewis acid site.The research results provide a theoretical basis for the preparation of efficient and inexpensive Fe-based catalysts from MD.展开更多
As one of the most important chemicals and carbon-free energy carriers,ammonia(NH3)has significant energy-related applications in industry and agriculture.Ninety percent of NH_(3) is produced by the Haber-Bosch proces...As one of the most important chemicals and carbon-free energy carriers,ammonia(NH3)has significant energy-related applications in industry and agriculture.Ninety percent of NH_(3) is produced by the Haber-Bosch process using high-purity N_(2) and H_(2) at high temperatures and pressures,which consumes about 1%of the total energy production and causes 1.4% of global CO_(2) emissions.The environmentally friendly electrochemical nitrogen reduction reaction(NRR)with low energy consumption is a promising alternative to the conventional Haber-Bosch process.However,the main issue is the low Faradaic efficiency and NH3 selectivity of electrochemical NRR,caused by inert nitrogen molecules and competitive hydrogen evolution reaction.As one of the cheapest and most abundant transition metals widely utilized in the Haber-Bosch process,the Fe element has presented the potential high performance for the electrochemical NRR.This article summarizes recent advances and research progress in non-noble Fe-based catalysts used for NH_(3) electrosynthesis.Various synthetic protocols,structure/morphology modification,performance improvement,and reaction mechanisms are comprehensively presented.Based on recent experimental and theoretical studies,we aim to illuminate the structure-property relationship and offer an excellent opportunity for engineering advanced Fe-based catalysts for nitrogen fixation.The most critical challenges and opportunities for Fe-based catalysts are also provided.This review would open up a promising avenue toward developing platinum-group-metal-free catalysts for electrochemical NRR applications in the future.展开更多
Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespr...Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.展开更多
The design of efficient and robust non-precious metal electrocatalysts towards oxygen evolution reaction(OER)is of great value for developing green energy technologies.The in-situ formed high-valence(oxy)hydroxides sp...The design of efficient and robust non-precious metal electrocatalysts towards oxygen evolution reaction(OER)is of great value for developing green energy technologies.The in-situ formed high-valence(oxy)hydroxides species during the reconstruction process of pre-catalysts are recognized as the real contributing sites for OER.However,pre-catalysts generally undergo a slow and inadequate self-reconstruction.Herein,we reported a PO^(3-)_(4)optimized CoFe-based OER catalysts with amorphous structure,which enables a fast and deep reconstruction during the OER process.The amorphous structure induced by ligands PO^(3-)_(4)is prone to evolution and further form active species for OER.The electron interaction between metal sites can be modulated by electron-rich PO^(3-)_(4),which promotes generation of high active CoOOH.Simultaneously,the etching of PO^(3-)_(4)from the pre-catalysts during the catalytic process is in favor of accelerating the self-reconstruction.As a result,as-prepared precatalyst can generate high active CoOOH at a low potential of 1.4 V and achieve an in-depth reconstructed nanosheet structure with abundant OER active sites.Our work provides a promising design of pre-catalysts for realizing efficient catalysis of water oxidation.展开更多
The performance of proton exchange membrane fuel cells depends heavily on the oxygen reduction reaction(ORR)at the cathode,for which platinum-based catalysts are currently the standard.The high cost and limited availa...The performance of proton exchange membrane fuel cells depends heavily on the oxygen reduction reaction(ORR)at the cathode,for which platinum-based catalysts are currently the standard.The high cost and limited availability of platinum have driven the search for alternative catalysts.While FeN4 single-atom catalysts have shown promising potential,their ORR activity needs to be further enhanced.In contrast,dual-atom catalysts(DACs)offer not only higher metal loading but also the ability to break the ORR scaling relations.However,the diverse local structures and tunable coordination environments of DACs create a vast chemical space,making large-scale computational screening challenging.In this study,we developed a graph neural network(GNN)-based framework to predict the ORR activity of Fe-based DACs,effectively addressing the challenges posed by variations in local catalyst structures.Our model,trained on a dataset of 180 catalysts,accurately predicted the Gibbs free energy of ORR intermediates and overpotentials,and identified 32 DACs with superior catalytic activity compared to FeN4 SAC.This approach not only advances the design of high-performance DACs,but also offers a powerful computational tool that can significantly reduce the time and cost of catalyst development,thereby accelerating the commercialization of fuel cell technologies.展开更多
Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal int...Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.展开更多
S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB...S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.展开更多
Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by ...Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.展开更多
Catalytic decomposition of methane using a Fe-based catalyst for hydrogen production has been studied in this work. A Fe/Al2O3 catalyst previously developed by our research group has been tested in a fluidized bed rea...Catalytic decomposition of methane using a Fe-based catalyst for hydrogen production has been studied in this work. A Fe/Al2O3 catalyst previously developed by our research group has been tested in a fluidized bed reactor （FBR）. A parametric study ot the effects of some process variables, including reaction temperature and space velocity, is undertaken. The operating conditions strongly affect the catalyst performance. Methane conversion was increased by increasing the temperature and lowering the space velocity. Using temperatures between 700 and 900℃ and space velocities between 3 and 6 LN/（gcat·h）, a methane conversion in the range of 25%-40% for the gas exiting the reactor could be obtained during a 6 h run. In addition, carbon was deposited in the form of nanofilaments （chain like nanofibers and multiwall nanotubes） with similar properties to those obtained in a fixed bed reactor.展开更多
Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cath...Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cathode materials influence the cost and energy output of SIBs.Therefore,the development of advanced cathode materials is crucial for the practical application of SIBs.Among various cathode materials,layered transition metal oxides(LTMOs)have received widespread attention owing to their straightforward preparation,abundant availability,and cost-competitiveness.Notably,layered Fe-based oxide cathodes are deemed to be one of the most promising candidates for the lowest price and easy-to-improve performance.Nevertheless,the challenges such as severe phase transitions,sluggish diffusion kinetics and interfacial degradation pose significant hurdles in achieving high-performance cathodes for SIBs.This review first briefly outlines the classification of layered structures and the working principle of layered oxides.Then,recent advances in modification strategies employed to address current issues with layered iron-based oxide cathodes are systematically reviewed,including ion doping,biphasic engineering and surface modification.Furthermore,the review not only outlines the prospects and development directions for layered Fe-based oxide cathodes but also provides novel insights and directions for future research endeavors for SIBs.展开更多
The alteration and formation of toxic compounds and potential changes in the toxicity of emissions when using after-treatment technologies have gained wide attention. Volatile organic compound（VOC）, carbonyl compoun...The alteration and formation of toxic compounds and potential changes in the toxicity of emissions when using after-treatment technologies have gained wide attention. Volatile organic compound（VOC）, carbonyl compound and particle-phase polycyclic aromatic hydrocarbon（PAH） emissions were tested at European Steady State Cycle（ESC） to study unregulated emissions from a diesel engine with a fuel-borne catalyst and diesel particulate filter（FBC–DPF）. An Fe-based fuel-borne catalyst was used for this study. According to the results, brake specific emissions of total VOCs without and with DPF were 4.7 and4.9 mg/kWh, respectively, showing a 4.3% increase. Benzene and n-undecane emissions increased and toluene emission decreased, while other individual VOC emissions basically had no change. When retrofitted with the FBC–DPF, total carbonyl compound emission decreased 15.7%, from 25.8 to 21.8 mg/kWh. The two highest carbonyls, formaldehyde and acetaldehyde, were reduced from 20.0 and 3.7 to 16.5 and 3.3 mg/kWh respectively. The specific reactivity（SR） with DPF was reduced from 6.68 to 6.64 mg/kWh. Total particle-phase PAH emissions decreased 66.4% with DPF compared to that without DPF. However, the Benzo[a]pyrene equivalent（BaPeq） with DPF had increased from 0.016 to 0.030 mg/kWh.Fluoranthene and Pyrene had the greatest decrease, 91.1% and 88.4% respectively. The increase of two- and three-ring PAHs with DPF indicates that the fuel-borne catalyst caused some gas-phase PAHs to adsorb on particles. The results of this study expand the knowledge of the effects of using a particulate filter and a Fe-based fuel-borne catalyst on diesel engine unregulated emissions.展开更多
Ni-based catalysts are widely applied in the hydrodeoxygenation of lignin derivatives via C-O cleavage for the production of cycloalkanes.However,they often have difficulty in achieving high activity under mild condit...Ni-based catalysts are widely applied in the hydrodeoxygenation of lignin derivatives via C-O cleavage for the production of cycloalkanes.However,they often have difficulty in achieving high activity under mild conditions and exhibit relatively poor stability,and rare studies focus on the cleavage of the stubborn interunit C-C linkages.To address this issue,we developed a Ni@AlPO_(4)/Al_(2)O_(3)catalyst in which the surface of Ni nanoparticles was decorated by AlPO_(4)species,demonstrating excellent catalytic activity and stability in the C-C and C-O cleavages.In the hydrodeoxygenation of guaiacol,this catalyst afforded99.1%conversion and 92.9%yield of cyclohexane under 1 MPa H_(2)at 230℃ for 2 h.More important,this catalyst maintained unchanged performance even after 6 runs with the conversion controlled at about50%,Mecha nistic investigations revealed that the moderate surface coverage of AlPO_(4)on Ni with the formation of Ni^(δ+)-AlPO_(4)interface significantly facilitated the conversion of methoxycyclohexanol and cyclohexanol to cyclohexane,whereas,excess coverage would also block the access to Ni site.Moreover,Ni@AlPO_(4)/Al_(2)O_(3)demonstrated broad applicability in the C-O cleavage of various typical lignin monomers and dimers into cycloalkanes.To our delight,this catalyst also displayed pretty good activity even in the simultaneous cleavage of C-C linkages and C-O bonds for the lignin-derived C-C dimers,achieving cycloalkanes as final products.As a consequence,a 27.1 wt%yield of monocycloalkanes was obtained in the depolymerization of poplar lignin with both C-C and C-O cleavages.展开更多
Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-perform...Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.展开更多
Novel hydrogen storage materials have propelled progress in hydrogen storage technologies.Magnesium hydride(MgH_(2))is a highly promising candidate.Nevertheless,several drawbacks,including the need for elevated therma...Novel hydrogen storage materials have propelled progress in hydrogen storage technologies.Magnesium hydride(MgH_(2))is a highly promising candidate.Nevertheless,several drawbacks,including the need for elevated thermal conditions,sluggish dehydrogena-tion kinetics,and high thermodynamic stability,limit its practical application.One effective method of addressing these challenges is cata-lyst doping,which effectively boosts the hydrogen storage capability of Mg-based materials.Herein,we review recent advancements in catalyst-doped MgH_(2) composites,with particular focus on multicomponent and high-entropy catalysts.Structure-property relationships and catalytic mechanisms in these doping strategies are also summarized.Finally,based on existing challenges,we discuss future research directions for the development of Mg-based hydrogen storage systems.展开更多
To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of cha...To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of characterization tests and evaluated the soot catalytic activity of the composite catalyst by comparing it with the LaCoO_(3) group,LaFeO_(3) group,and catalyst-free group.The results indicate that the Ag-LSCF composite catalyst exhibits the highest soot catalytic activity,with the characteristic temperature values of 376.3,431.1,and 473.9℃at 10%,50%,and 90%carbon soot conversion,respectively.These values are 24.8,20.2,and 23.1℃lower than those of the LSCF group.This also shows that LSCF can improve the catalytic activity of soot after compounding with Ag,and reflects the necessity of using catalysts in soot combustion reaction.XPS characterization and BET test show that Ag-LSCF has more abundant surface-adsorbed oxygen species,larger specific surface area and pore volume than LSCF,which also proves that Ag-LSCF has higher soot catalytic activity.展开更多
The influence of several anions on Fe-based Fischer-Tropsch catalyst, used in the synthesis of light olefins from synthesis gas, was studied. The results indicated that the addition of anions resulted in the reduction...The influence of several anions on Fe-based Fischer-Tropsch catalyst, used in the synthesis of light olefins from synthesis gas, was studied. The results indicated that the addition of anions resulted in the reduction of catalytic activity. When the anion content in the catalyst was 500 ppm, the influence of different anions on the catalysis activity was as follows： S^2- 〉Cl^-〉SO4^2-〉NO3. The addition of S^2- improved the selectivity of total hydrocarbons in the products, and Cl^- reduced this selectivity but increased the olefin content in the total hydrocarbons at the same time. When the contents of S^2- and Clin the catalyst were less than 50 ppm, their influence could be ignored. The XRD results indicated that the addition of anions reduced the contents of α-Fe and FeaC, which were the active components in the catalyst.展开更多
基金the Haihe Laboratory of Sus-tainable Chemical Transformations for financial support(No.24HHWCSS00009).
文摘Ammonia is essential for agriculture and,as a next-generation carbon-free fuel,typically produced through the Haber-Bosch method.This process requires high temperature and pressure,leading to significant energy consumption and greenhouse gas emissions.Therefore,achieving ammonia synthesis under milder conditions has been a long-standing goal.In this study,we design and synthesize a series of CeO_(2)-modified Fe/carbon-based catalysts with varying amounts of CeO_(2)(Ce_(x)Fe_(y)/C).The catalyst Ce_(2)Fe_(5)/C demonstrates an ammonia yield rate of 3.5 mmol/(g·h),which is 44 times greater than that of Fe/C and 8 times greater than that of commercial Fe-based catalysts at 300℃and 1 MPa.Temperature-programmed desorption experiments show that Ce_(2)Fe_(5)/C has enhanced nitrogen adsorption capabilities.Multiple analyses confirm that the CeO_(2)in Ce_(2)Fe_(5)/C is rich in oxygen vacancies,which can provide electrons to Fe,facilitating nitrogen adsorption,dissociation,and activity in low-temperature ammonia synthesis.
基金supported by the Ministry of Higher Education,Science and Innovation,and the Slovenian Research Agency(ARIS)throughresearch grants J7-4638 and J2-4441.
文摘The development of human industry inevitably leads to excessive carbon dioxide(CO_(2))emissions.It can cause critical ecological consequences,primarily global warming and ocean acidification.In this regard,close attention is paid to the carbon capture,utilization,and storage concept.The key component of this concept is the catalytic conversion of CO_(2)into valuable chemical compounds and fuels.Light olefins are one of the most industrially important chemicals,and their sustainable production via CO_(2)hydrogenation could be a prospective way to reach carbon neutrality.Fe-based materials are widely recognized as effective thermocatalysts and photothermal catalysts for that process thanks to their low cost,high activity,and good stability.This review critically examines the most recent progress in the development and optimization of Fe-based catalysts for CO_(2)hydrogenation into light olefins.Particular attention is paid to understanding the roles of catalyst composition,structural properties,and promoters in enhancing catalytic activity,selectivity,and stability.
基金financially supported by the National Key R&D Program of China (2023YFB4104501)the National Natural Science Foundation of China (22372165)+2 种基金the Liaoning Binhai Laboratory (LBLA-2024-01)the Grant. YLU-DNL Fund (2023001)DICP (Grant: DICP I202457)
文摘Regulating the location of the metal promoters plays a vital role in catalyst structure and its catalytic behavior during CO_(2)hydrogenation to higher alcohols.Herein,we selected the metal promoters with a precipitation pH similar to that of Cu^(2+)or Fe^(3+)to prepare a series of CuFe-based catalysts.Characterization results show that doping Al or Cr promoter,located with the Fe phase,suppressed the excessive carburization of the Fe phase and maintained an optimal proportion between Fe_(3)O_(4) and amorphous iron carbide(FeC_(x)),thus exhibiting superior catalytic activity and stability.In contrast,doping Zn or In promoter,located with the Cu phase,underwent a deeper carburization and formed more crys-talline FeC_(x),showing an inferior performance.The CuFeCr catalyst achieved the highest space-time yield of 330 mg g_(cat)^(-1)h^(-1)for higher alcohols among these catalysts.This study provides a novel strategy for opti-mizing the structure of the active phases for CO_(2)hydrogenation.
基金supported by the Key Project of Natural Science Foundation of Ningxia(NZ13010)the National Natural Science Foundation of China(21366025)~~
文摘Fe‐based catalysts for the production of light olefins via the Fischer‐Tropsch synthesis were modi‐fied by adding a Zn promoter using both microwave‐hydrothermal and impregnation methods. The physicochemical properties of the resulting catalysts were determined by scanning electron mi‐croscopy, the Brunauer‐Emmett‐Teller method, X‐ray diffraction, H2 temperature‐programed re‐duction and X‐ray photoelectron spectroscopy. The results demonstrate that the addition of a Zn promoter improves both the light olefin selectivity over the catalyst and the catalyst stability. The catalysts prepared via the impregnation method, which contain greater quantities of surface ZnO, exhibit severe carbon deposition following activity trials. In contrast, those materials synthesized using the microwave‐hydrothermal approach show improved dispersion of Zn and Fe phases and decreased carbon deposition, and so exhibit better CO conversion and stability.
基金The research was financially sponsored by the Major Scientific Research Planning Project of Colleges and Universities in Anhui Province(Grant No.2023AH040147)the National Natural Science Foundation of China(Grant No.52074093)the Outstanding Youth Scientific Research Project of Colleges and Universities in Anhui Province(Grant No.2022AH030044).
文摘Metallurgical dust(MD)was used as raw material to prepare rare earth Ce-doped Fe-based catalysts.The results show that the Ce_(0.1)/AMD-300℃catalyst prepared from acid-modified diatomite(AMD)with mCe/mMD=0.1(m_(Ce)and m_(MD)are the mass of Ce and MD,respectively)after being roasted at 300℃can reach 99%NO_(x)removal rate in the wide temperature range of 230–430℃and exhibits excellent So_(2)and H_(2)o resistance.The MD effectively removes alkali metal elements by the modification process,increases the specific surface area and optimizes the pore structure of MD.The doping of Ce element makes Fe-based catalysts have more surface adsorbed oxygen O_(α)and a higher Ce^(3+)/Ce^(4+)ratio.Through ammonia temperature-programmed desorption and hydrogen temperature-programmed reduction,it was found that the strong interaction between cerium and iron promotes the formation of more oxygen cavities in the catalyst,thereby generating more active and easily reducible oxygen species and promoting the transformation of Brønsted acid site to Lewis acid site.The research results provide a theoretical basis for the preparation of efficient and inexpensive Fe-based catalysts from MD.
基金National Natural Science Foundation of China,Grant/Award Numbers:21902021,21908017Fundamental Research Funds for the Central Universities,Grant/Award Numbers:DUT20RC(4)020,DUT20RC(4)018+1 种基金Open Foundation of Key Laboratory of Industrial Ecology and Environmental Engineering,Grant/Award Numbers:KLIEEE-20-01,KLIEEE-21-02Supercomputing Center of Dalian University of Technology。
文摘As one of the most important chemicals and carbon-free energy carriers,ammonia(NH3)has significant energy-related applications in industry and agriculture.Ninety percent of NH_(3) is produced by the Haber-Bosch process using high-purity N_(2) and H_(2) at high temperatures and pressures,which consumes about 1%of the total energy production and causes 1.4% of global CO_(2) emissions.The environmentally friendly electrochemical nitrogen reduction reaction(NRR)with low energy consumption is a promising alternative to the conventional Haber-Bosch process.However,the main issue is the low Faradaic efficiency and NH3 selectivity of electrochemical NRR,caused by inert nitrogen molecules and competitive hydrogen evolution reaction.As one of the cheapest and most abundant transition metals widely utilized in the Haber-Bosch process,the Fe element has presented the potential high performance for the electrochemical NRR.This article summarizes recent advances and research progress in non-noble Fe-based catalysts used for NH_(3) electrosynthesis.Various synthetic protocols,structure/morphology modification,performance improvement,and reaction mechanisms are comprehensively presented.Based on recent experimental and theoretical studies,we aim to illuminate the structure-property relationship and offer an excellent opportunity for engineering advanced Fe-based catalysts for nitrogen fixation.The most critical challenges and opportunities for Fe-based catalysts are also provided.This review would open up a promising avenue toward developing platinum-group-metal-free catalysts for electrochemical NRR applications in the future.
基金supports from the National Natural Science Foundation of China(Grant Nos.12305372 and 22376217)the National Key Research&Development Program of China(Grant Nos.2022YFA1603802 and 2022YFB3504100)+1 种基金the projects of the key laboratory of advanced energy materials chemistry,ministry of education(Nankai University)key laboratory of Jiangxi Province for persistent pollutants prevention control and resource reuse(2023SSY02061)are gratefully acknowledged.
文摘Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.
基金financially supported by the National Natural Science Foundation of China (Grants Nos.51772338,51972349,91963210 and U1801255).
文摘The design of efficient and robust non-precious metal electrocatalysts towards oxygen evolution reaction(OER)is of great value for developing green energy technologies.The in-situ formed high-valence(oxy)hydroxides species during the reconstruction process of pre-catalysts are recognized as the real contributing sites for OER.However,pre-catalysts generally undergo a slow and inadequate self-reconstruction.Herein,we reported a PO^(3-)_(4)optimized CoFe-based OER catalysts with amorphous structure,which enables a fast and deep reconstruction during the OER process.The amorphous structure induced by ligands PO^(3-)_(4)is prone to evolution and further form active species for OER.The electron interaction between metal sites can be modulated by electron-rich PO^(3-)_(4),which promotes generation of high active CoOOH.Simultaneously,the etching of PO^(3-)_(4)from the pre-catalysts during the catalytic process is in favor of accelerating the self-reconstruction.As a result,as-prepared precatalyst can generate high active CoOOH at a low potential of 1.4 V and achieve an in-depth reconstructed nanosheet structure with abundant OER active sites.Our work provides a promising design of pre-catalysts for realizing efficient catalysis of water oxidation.
基金This work was supported by the National Natural Science Foundation of China(No.22473001)the Natural Science Funds for Distinguished Young Scholar of Anhui Province(1908085J08)the University An-nual Scientific Research Plan of Anhui Province(2022AH010013).
文摘The performance of proton exchange membrane fuel cells depends heavily on the oxygen reduction reaction(ORR)at the cathode,for which platinum-based catalysts are currently the standard.The high cost and limited availability of platinum have driven the search for alternative catalysts.While FeN4 single-atom catalysts have shown promising potential,their ORR activity needs to be further enhanced.In contrast,dual-atom catalysts(DACs)offer not only higher metal loading but also the ability to break the ORR scaling relations.However,the diverse local structures and tunable coordination environments of DACs create a vast chemical space,making large-scale computational screening challenging.In this study,we developed a graph neural network(GNN)-based framework to predict the ORR activity of Fe-based DACs,effectively addressing the challenges posed by variations in local catalyst structures.Our model,trained on a dataset of 180 catalysts,accurately predicted the Gibbs free energy of ORR intermediates and overpotentials,and identified 32 DACs with superior catalytic activity compared to FeN4 SAC.This approach not only advances the design of high-performance DACs,but also offers a powerful computational tool that can significantly reduce the time and cost of catalyst development,thereby accelerating the commercialization of fuel cell technologies.
基金financially supported by the National Natural Science Foundation of China(22309137,22279095)Open subject project State Key Laboratory of New Textile Materials and Advanced Processing Technologies(FZ2023001).
文摘Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.
基金financially supported by the National Natural Science Foundation of China(Nos.51602018 and 51902018)the Natural Science Foundation of Beijing Municipality(No.2154052)+3 种基金the China Postdoctoral Science Foundation(No.2014M560044)the Fundamental Research Funds for the Central Universities(No.FRF-MP-20-22)USTB Research Center for International People-to-people Exchange in Science,Technology and Civilization(No.2022KFYB007)Education and Teaching Reform Foundation at University of Science and Technology Beijing(Nos.2023JGC027,KC2022QYW06,and KC2022TS09)。
文摘S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.
基金support from the Czech Science Foundation,project EXPRO,No 19-27454Xsupport by the European Union under the REFRESH—Research Excellence For Region Sustainability and High-tech Industries project number CZ.10.03.01/00/22_003/0000048 via the Operational Programme Just Transition from the Ministry of the Environment of the Czech Republic+1 种基金Horizon Europe project EIC Pathfinder Open 2023,“GlaS-A-Fuels”(No.101130717)supported from ERDF/ESF,project TECHSCALE No.CZ.02.01.01/00/22_008/0004587).
文摘Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.
基金the Spanish Science and InnovationMinistry for the financial support of Project ENE2008-06516-C03-01
文摘Catalytic decomposition of methane using a Fe-based catalyst for hydrogen production has been studied in this work. A Fe/Al2O3 catalyst previously developed by our research group has been tested in a fluidized bed reactor （FBR）. A parametric study ot the effects of some process variables, including reaction temperature and space velocity, is undertaken. The operating conditions strongly affect the catalyst performance. Methane conversion was increased by increasing the temperature and lowering the space velocity. Using temperatures between 700 and 900℃ and space velocities between 3 and 6 LN/（gcat·h）, a methane conversion in the range of 25%-40% for the gas exiting the reactor could be obtained during a 6 h run. In addition, carbon was deposited in the form of nanofilaments （chain like nanofibers and multiwall nanotubes） with similar properties to those obtained in a fixed bed reactor.
基金supported by the National Natural Science Foundation of China(no.52374301)the Open Project of Guangxi Key Laboratory of Electrochemical Energy Materials(no.GXUEEM2024001)+2 种基金the Hebei Provincial Natural Science Foundation(no.E2024501010)the Shijiazhuang Basic Research Project(no.241790667A)the Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(no.22567627H)。
文摘Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cathode materials influence the cost and energy output of SIBs.Therefore,the development of advanced cathode materials is crucial for the practical application of SIBs.Among various cathode materials,layered transition metal oxides(LTMOs)have received widespread attention owing to their straightforward preparation,abundant availability,and cost-competitiveness.Notably,layered Fe-based oxide cathodes are deemed to be one of the most promising candidates for the lowest price and easy-to-improve performance.Nevertheless,the challenges such as severe phase transitions,sluggish diffusion kinetics and interfacial degradation pose significant hurdles in achieving high-performance cathodes for SIBs.This review first briefly outlines the classification of layered structures and the working principle of layered oxides.Then,recent advances in modification strategies employed to address current issues with layered iron-based oxide cathodes are systematically reviewed,including ion doping,biphasic engineering and surface modification.Furthermore,the review not only outlines the prospects and development directions for layered Fe-based oxide cathodes but also provides novel insights and directions for future research endeavors for SIBs.
基金financial support from the National Natural Science Foundation of China (No. 51276021)the Development Projects of Shandong Province Science and Technology (No. 2011YD17001)
文摘The alteration and formation of toxic compounds and potential changes in the toxicity of emissions when using after-treatment technologies have gained wide attention. Volatile organic compound（VOC）, carbonyl compound and particle-phase polycyclic aromatic hydrocarbon（PAH） emissions were tested at European Steady State Cycle（ESC） to study unregulated emissions from a diesel engine with a fuel-borne catalyst and diesel particulate filter（FBC–DPF）. An Fe-based fuel-borne catalyst was used for this study. According to the results, brake specific emissions of total VOCs without and with DPF were 4.7 and4.9 mg/kWh, respectively, showing a 4.3% increase. Benzene and n-undecane emissions increased and toluene emission decreased, while other individual VOC emissions basically had no change. When retrofitted with the FBC–DPF, total carbonyl compound emission decreased 15.7%, from 25.8 to 21.8 mg/kWh. The two highest carbonyls, formaldehyde and acetaldehyde, were reduced from 20.0 and 3.7 to 16.5 and 3.3 mg/kWh respectively. The specific reactivity（SR） with DPF was reduced from 6.68 to 6.64 mg/kWh. Total particle-phase PAH emissions decreased 66.4% with DPF compared to that without DPF. However, the Benzo[a]pyrene equivalent（BaPeq） with DPF had increased from 0.016 to 0.030 mg/kWh.Fluoranthene and Pyrene had the greatest decrease, 91.1% and 88.4% respectively. The increase of two- and three-ring PAHs with DPF indicates that the fuel-borne catalyst caused some gas-phase PAHs to adsorb on particles. The results of this study expand the knowledge of the effects of using a particulate filter and a Fe-based fuel-borne catalyst on diesel engine unregulated emissions.
基金supported by National Natural Science Foundation of China(22178258,22308254)China Postdoctoral Science Foundation(2023M742593,2024T170642)+1 种基金Independent Innova-tion Fund of Tianjin University(2024XQM-0021)the Open Fund of the Key Laboratory of Functional Molecular Solids(FMS2023006)。
文摘Ni-based catalysts are widely applied in the hydrodeoxygenation of lignin derivatives via C-O cleavage for the production of cycloalkanes.However,they often have difficulty in achieving high activity under mild conditions and exhibit relatively poor stability,and rare studies focus on the cleavage of the stubborn interunit C-C linkages.To address this issue,we developed a Ni@AlPO_(4)/Al_(2)O_(3)catalyst in which the surface of Ni nanoparticles was decorated by AlPO_(4)species,demonstrating excellent catalytic activity and stability in the C-C and C-O cleavages.In the hydrodeoxygenation of guaiacol,this catalyst afforded99.1%conversion and 92.9%yield of cyclohexane under 1 MPa H_(2)at 230℃ for 2 h.More important,this catalyst maintained unchanged performance even after 6 runs with the conversion controlled at about50%,Mecha nistic investigations revealed that the moderate surface coverage of AlPO_(4)on Ni with the formation of Ni^(δ+)-AlPO_(4)interface significantly facilitated the conversion of methoxycyclohexanol and cyclohexanol to cyclohexane,whereas,excess coverage would also block the access to Ni site.Moreover,Ni@AlPO_(4)/Al_(2)O_(3)demonstrated broad applicability in the C-O cleavage of various typical lignin monomers and dimers into cycloalkanes.To our delight,this catalyst also displayed pretty good activity even in the simultaneous cleavage of C-C linkages and C-O bonds for the lignin-derived C-C dimers,achieving cycloalkanes as final products.As a consequence,a 27.1 wt%yield of monocycloalkanes was obtained in the depolymerization of poplar lignin with both C-C and C-O cleavages.
基金supported by the National Natural Science Foundation of China(No.21571062)the Program for Professor of Special Appointment(Eastern Scholar)at the Shanghai Institutions of Higher Learning to JGL,and the Fundamental Research Funds for the Central Universities(No.222201717003)。
文摘Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
基金financially supported by the National Key Research and Development Program of China (No. 2021YFB4000604)the National Natural Science Foundation of China (No. 52271220)+2 种基金the 111 Project (No. B12015)the Fundamental Research Funds for the Central UniversitiesHaihe Laboratory of Sustainable Chemical Transformations, Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Materials, Science Research and Technology Development Project of Guilin (No. 20210102-4)
文摘Novel hydrogen storage materials have propelled progress in hydrogen storage technologies.Magnesium hydride(MgH_(2))is a highly promising candidate.Nevertheless,several drawbacks,including the need for elevated thermal conditions,sluggish dehydrogena-tion kinetics,and high thermodynamic stability,limit its practical application.One effective method of addressing these challenges is cata-lyst doping,which effectively boosts the hydrogen storage capability of Mg-based materials.Herein,we review recent advancements in catalyst-doped MgH_(2) composites,with particular focus on multicomponent and high-entropy catalysts.Structure-property relationships and catalytic mechanisms in these doping strategies are also summarized.Finally,based on existing challenges,we discuss future research directions for the development of Mg-based hydrogen storage systems.
文摘To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of characterization tests and evaluated the soot catalytic activity of the composite catalyst by comparing it with the LaCoO_(3) group,LaFeO_(3) group,and catalyst-free group.The results indicate that the Ag-LSCF composite catalyst exhibits the highest soot catalytic activity,with the characteristic temperature values of 376.3,431.1,and 473.9℃at 10%,50%,and 90%carbon soot conversion,respectively.These values are 24.8,20.2,and 23.1℃lower than those of the LSCF group.This also shows that LSCF can improve the catalytic activity of soot after compounding with Ag,and reflects the necessity of using catalysts in soot combustion reaction.XPS characterization and BET test show that Ag-LSCF has more abundant surface-adsorbed oxygen species,larger specific surface area and pore volume than LSCF,which also proves that Ag-LSCF has higher soot catalytic activity.
文摘The influence of several anions on Fe-based Fischer-Tropsch catalyst, used in the synthesis of light olefins from synthesis gas, was studied. The results indicated that the addition of anions resulted in the reduction of catalytic activity. When the anion content in the catalyst was 500 ppm, the influence of different anions on the catalysis activity was as follows： S^2- 〉Cl^-〉SO4^2-〉NO3. The addition of S^2- improved the selectivity of total hydrocarbons in the products, and Cl^- reduced this selectivity but increased the olefin content in the total hydrocarbons at the same time. When the contents of S^2- and Clin the catalyst were less than 50 ppm, their influence could be ignored. The XRD results indicated that the addition of anions reduced the contents of α-Fe and FeaC, which were the active components in the catalyst.
