The 70th anniversary of Dalian Institute of Chemical Physics(DICP),Chinese Academy of Sciences(CAS),has been celebrating in various ways through the year of 2019.DICP was established with the name of Scientific Resear...The 70th anniversary of Dalian Institute of Chemical Physics(DICP),Chinese Academy of Sciences(CAS),has been celebrating in various ways through the year of 2019.DICP was established with the name of Scientific Research Institute of Dalian University on March 19,1949,which is even a little earlier than the foundation of the People's Republic of China(October 1,1949).Since then,the name of the institute has changed several times in order to fulfill the assigned regional and national research mission.In 1970,the institute was named as the“Dalian Institute of Chemical Physics,Chinese Academy of Sciences”.展开更多
Dalian Institute of Chemical Physics(DICP) is a comprehensive chemical engineering research institute with strong international reputation, which has made significant contributions to national economic construction, n...Dalian Institute of Chemical Physics(DICP) is a comprehensive chemical engineering research institute with strong international reputation, which has made significant contributions to national economic construction, national security and the progress of science and technology(S&T).展开更多
This article presents a history of the origins of the Dalian Institute of Chemical Physics, Chinese Academy of Sciences (Abbreviated as DICP) and relates the recent friendship between China and Japan in the field of c...This article presents a history of the origins of the Dalian Institute of Chemical Physics, Chinese Academy of Sciences (Abbreviated as DICP) and relates the recent friendship between China and Japan in the field of catalysis. Although the official beginning of DICP is in 1949 with the birth of the People’s Republic of China, there are earlier roots that went back to the defeat of Russia by Imperial Japan in 1905. This began a period of occupation and exploitation of Northest Asia by Japan which did not end until its defeat by Allied forces in 1945. During the period of occupation, a laboratory was created called the Central Research Laboratory of the South Manchurian Railroad Company, which was staffed by the best and brightest researchers from Japan, and was able to develop new processes in chemicals and synthetic fuels that fed the Japanese Imperial forces. Between 1945 and 1949, Dalian was administered by the Soviet Union, and the removable equipment from the Laboratory was taken. In this period one individual stood out, the Laboratory Director Marusawa Tsuneya, who risked his life to preserve the scientific records and staff of the institute, and then stayed in Dalian for ten years after the Second World War to help China rebuild its capabilities. The Central Research Laboratory is still preserved as the Old Campus of DICP.The origin of the friendship between China and Japan in catalysis can be traced to Professor Morikawa Kiyoshi, who worked in the Central Research Laboratory and helped commercialize a shale coal liquefaction process. Upon his return to Japan he became Professor at the Tokyo Institute of Technology and in 1975 organized the first visit by Japanese academics to China. This was reciprocated in visits to Japan in 1977 and 1980 by top researchers such as Zhang Dayu, Min Enze, Tsai Khirui, Lu Jiaxi, and Lin Liwu. This resulted in numerous contacts between individuals, which multiplied geometrically. Notably among these were the personal interactions between Guo Xiexian, the Vice-Director of DICP and Tamaru Kenzi, a Professor at the University of Tokyo, which led to a friendship lasting decades and encompassing generations. In 1981, Guo Xiexian organized the first China-Japan-USA Symposium in Dalian, assisted by Tamaru Kenzi, which was attended by over 90 scientists. This meeting was a big success, and was to lead to the organization of many other multi-country conferences, further promoting exchanges. It culminated with the hosting of China of the 16<sup>th</sup> International Congress on Catalysis in 2016 in Beijing, with Li Can as President.Today DICP is a sprawling organization with over 1300 permanent staff, and is one of the powerhouses of catalysis in the world. From 2000, it has been led by Directors Bao Xinhe, Zhang Tao, and Liu Zhongmin. The Institute is making enormous contributions to research and producing cutting-edge technology, and its future is bright.展开更多
Development of non-noble-metal electrocatalysts with robust oxygen evolution reaction(OER)at the industrially required current density is desirable but still lacking for promising industrial-scale water electrolysis.H...Development of non-noble-metal electrocatalysts with robust oxygen evolution reaction(OER)at the industrially required current density is desirable but still lacking for promising industrial-scale water electrolysis.Here,we report one cobalt phosphide-based heterostructure anode(denoted as Co_(x)P-HS hereafter)to exhibit extremely robust alkaline OER at 500 mA cm^(−2).Together with home-made NiMoOx cathode,we could fabricate one efficient two-electrode overall water splitting system,based on which one photovoltaic-driven electrochemical(PV-EC)water splitting device was further constructed for robust solar-to-hydrogen(STH)conversion with efficiency of over∼27.10%under one sun illumination.The extraordinary OER stability of our catalyst was unraveled to predominantly result from all-for-one design of multiple structural parameters,where the quasi-in situ growth of catalyst is favorable to prevent physical exfoliation of catalyst,while the local structure featured with two-dimensional morphology,polymorphic heterostructure and sulfur-doping modulation is highly desirable for efficient charge transfer and surface catalysis,leading to excellent electrochemical stability.展开更多
Pt-rare-earth(PtRE)alloys are considered to be highly promising catalysts for oxygen reduction reaction(ORR)in acidic electrolytes.However,the wet-chemical synthesis of PtRE nanoalloys still faces significant challeng...Pt-rare-earth(PtRE)alloys are considered to be highly promising catalysts for oxygen reduction reaction(ORR)in acidic electrolytes.However,the wet-chemical synthesis of PtRE nanoalloys still faces significant challenges.The precise reaction mechanism for ORR of these catalysts is still unclear on significant aspects involving the rate-determining step and the nature of the ligand effect.Herein,we report a class of solvothermal synthesis of PtRE(RE is Dy or La)nanoalloys.Such PtRE nanoalloys here are active and stable in acidic media,with both high mass activities enhanced by 2-5 times relative to commercial Pt/C catalyst and high stabilities indicative of the little activity decay and negligible structure change after 10,000 cycles.Density functional theory calculations firmly confirm that the ligand effect of RE elements accelerates an O-O bond scission and steers the rate-determining steps from OH^(*)+H^(+)+e-→H_(2)O(on pure Pt surface)to HOOH^(*)+H^(+)+e-→OH^(*)+H_(2)O(on the PtRE nanoalloy surface)for the fast reaction kinetics,which could be fine-tuned by regulating the RE electronic structures and consequently endows the maximal rate of ORR catalysis with PtDy alloy catalysts.展开更多
Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined acti...Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined active sites and high loadings under precise control has become a hotly debated topic in scientific research.Metal-organic frameworks(MOFs),with their exceptional properties such as ultrahigh specific surface areas,precisely controllable structural de-signs,and highly flexible functional cus-tomization capabilities,are regarded as one of the ideal matrices for supporting and sta-bilizing SACs.This review provides an in-sightful overview of the diverse preparation strategies for MOFs-derived SACs.It comprehen-sively analyzes the unique advantages and challenges of each method in achieving efficient synthesis of SACs,emphasizing the crucial role of optimized processes in unlocking the antici-pated performance of SACs.Furthermore,this review delves into a series of advanced charac-terization techniques,including aberration-corrected scanning transmission electron mi-croscopy(AC-STEM),electron energy loss spectroscopy(EELS),X-ray absorption spec-troscopy(XAS),and infrared absorption spectroscopy(IRAS),offering valuable insights into the atomic-scale fine structures and properties of SACs,significantly advancing the under-standing of SAC mechanisms.Moreover,this review focuses on exploring the potential appli-cations of MOFs-derived SACs in electrocatalysis frontier fields.This comprehensive exami-nation lays a solid theoretical foundation and provides a directional guidance for the rational design and controllable synthesis of high-performance MOFs-derived SACs.展开更多
Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and ca...Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.展开更多
In fulfillment of the national science-and-technology development agenda, the Department of Chemical Sciences of the National Natural Science Foundation of China (NSFC) convened the Strategic Symposium on the Fifteent...In fulfillment of the national science-and-technology development agenda, the Department of Chemical Sciences of the National Natural Science Foundation of China (NSFC) convened the Strategic Symposium on the Fifteenth FiveYear (20262030) Development Plan for Electrochemistry held in Xiamen on 29 August, 2025-the culminating year of the Fourteenth Five-Year (2021-2025) Development Plan. More than forty leading experts in the field of electrochemistry participated with spanning nine thematic fronts: Interfacial Electrocatalysis, Interfacial Electrochemistry for Energy Storage, Bioelectrochemistry, Electrochemistry of Hydrogen Energy, Electrochemical Micro-/Nano-Manufacturing, Operando Electrochemical Characterization, Electro-Thermal Coupling Catalysis, Theoretical and Computational Electrochemistry,and Electrochemical Synthesis. The forum assembled China's foremost electrochemical expertise to blueprint high-quality disciplinary growth for the coming five-year period, thereby serving overarching national strategic needs and sharpening the international competitiveness of Chinese electrochemistry.This paper is presented to highlight the strategic needs and priority areas for the next five years (2026-2030) based on this symposium. The development status of basic research and applied basic research in China's electrochemistry field is systematically reviewed. The in-depth analyses of the existing problems and key challenges in the research and development of electrochemistry related fields are outlined, and the frontier research areas and development trends in the next 5-10 years by integrating national major strategic needs are discussed, which will further promote the academic community to reach a clearer consensus. The proposed strategic roadmap is intended to accelerate a sharpened community consensus, propel the discipline toward high-quality advancement, and furnish a critical reference for building China into a world-leading science and technology power.展开更多
In response to the awareness of limited fossil resources and environmental concerns,catalytic conversion of renewable lignocellulose biomass to value-added chemicals and fuels is of great significance and attractive f...In response to the awareness of limited fossil resources and environmental concerns,catalytic conversion of renewable lignocellulose biomass to value-added chemicals and fuels is of great significance and attractive for sustainable chemistry.Division of Biomass Conversion and Bio-Energy attached to Dalian National Laboratory for Clean Energy has devoted themselves to valorization of lignocellulose biomass since launched in 2011.Our research interests focus on breeding of biomass resources(inulin and microalgae),exploration of catalytic and biological technologies,and production of energy chemicals and fuels.Although lignocellulose biomass is renewable and abundant,the way of utilization should be reasonable according to its structural characteristics in view of efficiency and economy.In this review,to celebrate the DICP's 70 th anniversary,we will highlight the major fundamental advances in DICP about the conversion of lignocellulose to value-added chemicals and liquid fuels.Particular attention will be paid to the transformation of cellulose and its derivatives to glycols,acids and nitrogen-containing chemicals,hemicellulose-derived platform molecule furfural to jet fuels and lignin to aromatics using catalytic technologies.展开更多
Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy.Precise synthesis of catalytically active nanostructures is one of the key challenge...Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy.Precise synthesis of catalytically active nanostructures is one of the key challenges that hinder the practical application of many important energy‐related electrocatalytic reactions.Compared with conventional wet‐chemical,solid‐state and vapor deposition synthesis,electrochemical synthesis is a simple,fast,cost‐effective and precisely controllable method for the preparation of highly efficient catalytic materials.In this review,we summarize recent progress in the electrochemical synthesis of catalytic materials such as single atoms,spherical and shaped nanoparticles,nanosheets,nanowires,core‐shell nanostructures,layered nanomaterials,dendritic nanostructures,hierarchically porous nanostructures as well as composite nanostructures.Fundamental aspects of electrochemical synthesis and several main electrochemical synthesis methods are discussed.Structure‐performance correlations between electrochemically synthesized catalysts and their unique electrocatalytic properties are exemplified using selected examples.We offer the reader with a basic guide to the synthesis of highly efficient catalysts using electrochemical methods,and we propose some research challenges and future opportunities in this field.展开更多
The concentration of polychlorinated biphenyls （PCBs） in the urban air of Dalian, China was monitored from November 2009 to October 2010 with active high-volume sampler and semipermeable membrane device （SPMD） pas...The concentration of polychlorinated biphenyls （PCBs） in the urban air of Dalian, China was monitored from November 2009 to October 2010 with active high-volume sampler and semipermeable membrane device （SPMD） passive sampler. The concentration of PCBs （particle ＋ gas） （∑PCBs） ranged from 18.6 to 91.0 pg/m3, with an average of 50.9 pg/m3, and the most abundant dioxin-like PCB （DL-PCBs） was PCB118. The WHO-TEQ values of DL-PCBs were 3.6--22.1 fg/m3, with an average of 8.5 fg/m3, and PCB126 was the maximum contributor to ZTEQ. There was a much larger amount of PCBs in the gas phase than in the particulate phase. The dominant PCB components were lower and middle molecular weight PCBs. With increasing chlorination level, the concentration of the PCB congeners in the air decreased. The gas-particulate partitioning of PCBs was different for the four seasons. The gas- particulate partitioning coefficients （logKp） vs. subcooled liquid vapor pressures （logPL~） of PCBs had reasonable correlations for different sampling sites and seasons. The absorption mechanism contributed more to the gas-particulate partitioning process than adsorption. Correlation analysis of meteorological parameters with the concentration of PCBs was conducted using SPSS packages. The ambient temperature and atmospheric pressure were important factors influencing the concentration of PCBs in the air. The distribution pattern of the congeners of PCBs and the dominant contributors to DL-PCBs and TEQ in active samples and SPMDs passive samples were similar. SPMD mainly sequestrated gas phase PCBs.展开更多
Electrochemical CO2 reduction to chemicals or fuels presents one of the most promising strategies for managing the global carbon balance, which yet poses a significant challenge due to lack of efficient and durable el...Electrochemical CO2 reduction to chemicals or fuels presents one of the most promising strategies for managing the global carbon balance, which yet poses a significant challenge due to lack of efficient and durable electrocatalyst as well as the understanding of the CO2 reduction reaction(CO2RR) mechanism.Benefiting from the large surface area, high electrical conductivity, and tunable structure, carbon-based metal-free materials(CMs) have been extensively studied as cost-effective electrocatalysts for CO2RR.The development of CMs with low cost, high activity and durability for CO2RR has been considered as one of the most active and competitive directions in electrochemistry and material science.In this review article,some up-to-date strategies in improving the CO2RR performance on CMs are summarized.Specifically, the approaches to optimize the adsorption of CO2RR intermediates, such as tuning the physical and electronic structure are introduced, which can enhance the electrocatalytic activity of CMs effectively.Finally, some design strategies are proposed to prepare CMs with high activity and selectivity for CO2RR.展开更多
The concentration of short-chain polychlorinated paraffins(SCCPs) in the urban air of Dalian,China was monitored from September 2016 to August 2017 with a self-developed passive sampler(PAS1) and an active high-volume...The concentration of short-chain polychlorinated paraffins(SCCPs) in the urban air of Dalian,China was monitored from September 2016 to August 2017 with a self-developed passive sampler(PAS1) and an active high-volume sampler, simultaneously. PAS1 successfully collected the entire target SCCPs in the ambient air. Air SCCPs sampled by PAS1 were found be in the linear uptake stage during 181 days of sampling. Passive and active samples showed comparable congener profiles, and the dominant contributors of SCCPs in the two kinds of samples were similar. A significant linear correlation was observed between the total concentration of SCCPs sampled by PAS1 and active sampler in the four seasons. The passive sampling rates of the PAS1 for the gas and particulate phases of SCCPs were measured. The quantitative structure–property relationship of the sampling rate of PAS1(Rair) for gas-phase SCCPs was studied. From the molecular point of view, Rairwas mainly affected by the molecular weight and sub-cooled liquid vapor pressure of SCCPs. In general, SCCPs in the urban air of Dalian mainly existed in gas phase,lower molecular weight SCCPs primarily occurred in the gas phase, whereas higher molecular weight SCCPs were predominately adsorbed or absorbed on airborne particles. The air concentration of SCCPs in the four seasons were different, the correlation of the concentration of SCCPs in the air with the meteorology parameters was conducted. The exposure risk by intake air SCCPs of the residents around the sampling sites was evaluated according to the European risk assessment standards.展开更多
The effort on electrochemical reduction of COto useful chemicals using the renewable energy to drive the process is growing fast recently. In this review, we introduce the recent progresses on the electrochemical redu...The effort on electrochemical reduction of COto useful chemicals using the renewable energy to drive the process is growing fast recently. In this review, we introduce the recent progresses on the electrochemical reduction of COin solid oxide electrolysis cells（SOECs）. At high temperature, only CO is produced with high current densities and Faradic efficiency while the reactor is complicated and a better sealing technique is urgently needed. The typical electrolytes such as zirconia-based oxides, ceria-based oxides and lanthanum gallates-based oxides, anodes and cathodes are introduced in this review, and the cathode materials, such as conventional metal–ceramics（cermets）, mixed ionic and electronic conductors（MIECs） are discussed in detail. In the future, to gain more value-added products, the electrolyte, cathode and anode materials should be developed to allow SOECs to be operated at temperature range of 573–873 K. At those temperatures, SOECs may combine the advantages of the low temperature system and the high temperature system to produce various products with high current densities.展开更多
In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a pro...In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.展开更多
The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this ...The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this field,the reported catalysts rarely deviate from the traditionally supported metal nanoparticle morphology,with the most simplistic method of enhancement being the addition of more metals to an already complex composition.Encapsulated catalysts,especially yolk@shell catalysts with hollow voids,offer answers to the most prominent issues faced by this field,coking and sintering,and further potential for more advanced phenomena,for example,the confinement effect,to promote selectivity or offer greater protection against coking and sintering.This work serves to demonstrate the current position of catalyst development in the fields of thermal CO_(2) reforming and hydrogenation,summarizing the most recent work available and most common metals used for these reactions,and how yolk@shell catalysts can offer superior performance and survivability in thermal CO_(2) reforming and hydrogenation to the more traditional structure.Furthermore,this work will briefly demonstrate the bespoke nature and highly variable yolk@shell structure.Moreover,this review aims to illuminate the spatial confinement effect and how it enhances yolk@shell structured nanoreactors is presented.展开更多
The methoxycarbonylations of cyclohexene and 1-decene with CO2 can take place under ambient conditions by catalysis of [Co]([Co]=Co(acac)(2), Co(OAc)(2), CoCl2) in the presence of ultraviolet irradiation.
Copper-indium bimetallic catalysts with a dendritic structure are fabricated by a two-step electrodeposition method using a hydrogen evolution template for the CO2 electroreduction reaction(CO2RR).The dendritic Cu-In-...Copper-indium bimetallic catalysts with a dendritic structure are fabricated by a two-step electrodeposition method using a hydrogen evolution template for the CO2 electroreduction reaction(CO2RR).The dendritic Cu-In-30 catalyst electrodeposited for 30 min shows the highest specific surface area and exposes the most active sites,resulting in improved CO2RR activity.The dendritic Cu-In-30 catalyst exhibits distinctly higher formate partial current density(42.0 m A cm^-2)and Faradaic efficiency(87.4%)than those of the In-30 catalyst without the dendritic structure(the formate partial current density and Faradaic efficiency are 4.6 m A cm^-2 and 57.0%,respectively)at-0.85 V vs.reversible hydrogen electrode,ascribed to the increased specific surface area.The Cu-In-30 catalyst can maintain stable performance for 12 h during the CO2RR.In addition,the intrinsic current density of Cu-In-30 with the dendritic structure(4.8 m A cm^-2)is much higher than that of In-30 without the dendritic structure(2.1 m A cm^-2),indicating that the dendritic structure promotes the CO2RR,possibly due to additional coordination unsaturated atoms.展开更多
The continuous wavelength chemical oxygen-iodine laser can be turned into pulse operation mode in order to obtain high energy and high pulse power. We propose an approach to produce iodine atoms instantaneously by pul...The continuous wavelength chemical oxygen-iodine laser can be turned into pulse operation mode in order to obtain high energy and high pulse power. We propose an approach to produce iodine atoms instantaneously by pulsed gas discharge with the assistance of spark pre-ionization to achieve the pulsed goal. The influence of spark pre-ionization on discharge homogeneity is discussed. Voltage-current characteristics are shown and discussed in existence of the pre-ionization capacitor and peaking capacitor. The spark pre-ionization and peaking capacitor are very helpful in obtaining a stable and homogeneous discharge. The lasing is achieved at the total pressure of 2.2-2.9 kPa and single pulse energy is up to 180 mJ, the corresponding specific output energy is 1.0 3/L.展开更多
The direct electrocatalytic synthesis of ammonia from N2 and H2O by using renewable energy sources and ambient pressure/temperature operations is a breakthrough technology,which can reduce by over 90%the greenhouse ga...The direct electrocatalytic synthesis of ammonia from N2 and H2O by using renewable energy sources and ambient pressure/temperature operations is a breakthrough technology,which can reduce by over 90%the greenhouse gas emissions of this chemical and energy storage process.We report here an in-situ electrochemical activation method to prepare Fe2O3-CNT(iron oxide on carbon nanotubes)electrocatalysts for the direct ammonia synthesis from N2 and H2O.The in-situ electrochemical activation leads to a large increase of the ammonia formation rate and Faradaic efficiency which reach the surprising high values of 41.6μg mgcat^−1 h^−1 and 17%,respectively,for an in-situ activation of 3 h,among the highest values reported so far for non-precious metal catalysts that use a continuous-flow polymer-electrolytemembrane cell and gas-phase operations for the ammonia synthesis hemicell.The electrocatalyst was stable at least 12 h at the working conditions.Tests by switching N2 to Ar evidence that ammonia was formed from the gas-phase nitrogen.The analysis of the changes of reactivity and of the electrocatalyst characteristics as a function of the time of activation indicates a linear relationship between the ammonia formation rate and a specific XPS(X-ray-photoelectron spectroscopy)oxygen signal related to O2−in iron-oxide species.This results together with characterization data by TEM and XRD suggest that the iron species active in the direct and selective synthesis of ammonia is a maghemite-type iron oxide,and this transformation from the initial hematite is responsible for the in-situ enhancement of 3-4 times of the TOF(turnover frequency)and NH3 Faradaic efficiency.This transformation is likely related to the stabilization of the maghemite species at CNT defect sites,although for longer times of preactivation a sintering occurs with a loss of performances.展开更多
文摘The 70th anniversary of Dalian Institute of Chemical Physics(DICP),Chinese Academy of Sciences(CAS),has been celebrating in various ways through the year of 2019.DICP was established with the name of Scientific Research Institute of Dalian University on March 19,1949,which is even a little earlier than the foundation of the People's Republic of China(October 1,1949).Since then,the name of the institute has changed several times in order to fulfill the assigned regional and national research mission.In 1970,the institute was named as the“Dalian Institute of Chemical Physics,Chinese Academy of Sciences”.
文摘Dalian Institute of Chemical Physics(DICP) is a comprehensive chemical engineering research institute with strong international reputation, which has made significant contributions to national economic construction, national security and the progress of science and technology(S&T).
文摘This article presents a history of the origins of the Dalian Institute of Chemical Physics, Chinese Academy of Sciences (Abbreviated as DICP) and relates the recent friendship between China and Japan in the field of catalysis. Although the official beginning of DICP is in 1949 with the birth of the People’s Republic of China, there are earlier roots that went back to the defeat of Russia by Imperial Japan in 1905. This began a period of occupation and exploitation of Northest Asia by Japan which did not end until its defeat by Allied forces in 1945. During the period of occupation, a laboratory was created called the Central Research Laboratory of the South Manchurian Railroad Company, which was staffed by the best and brightest researchers from Japan, and was able to develop new processes in chemicals and synthetic fuels that fed the Japanese Imperial forces. Between 1945 and 1949, Dalian was administered by the Soviet Union, and the removable equipment from the Laboratory was taken. In this period one individual stood out, the Laboratory Director Marusawa Tsuneya, who risked his life to preserve the scientific records and staff of the institute, and then stayed in Dalian for ten years after the Second World War to help China rebuild its capabilities. The Central Research Laboratory is still preserved as the Old Campus of DICP.The origin of the friendship between China and Japan in catalysis can be traced to Professor Morikawa Kiyoshi, who worked in the Central Research Laboratory and helped commercialize a shale coal liquefaction process. Upon his return to Japan he became Professor at the Tokyo Institute of Technology and in 1975 organized the first visit by Japanese academics to China. This was reciprocated in visits to Japan in 1977 and 1980 by top researchers such as Zhang Dayu, Min Enze, Tsai Khirui, Lu Jiaxi, and Lin Liwu. This resulted in numerous contacts between individuals, which multiplied geometrically. Notably among these were the personal interactions between Guo Xiexian, the Vice-Director of DICP and Tamaru Kenzi, a Professor at the University of Tokyo, which led to a friendship lasting decades and encompassing generations. In 1981, Guo Xiexian organized the first China-Japan-USA Symposium in Dalian, assisted by Tamaru Kenzi, which was attended by over 90 scientists. This meeting was a big success, and was to lead to the organization of many other multi-country conferences, further promoting exchanges. It culminated with the hosting of China of the 16<sup>th</sup> International Congress on Catalysis in 2016 in Beijing, with Li Can as President.Today DICP is a sprawling organization with over 1300 permanent staff, and is one of the powerhouses of catalysis in the world. From 2000, it has been led by Directors Bao Xinhe, Zhang Tao, and Liu Zhongmin. The Institute is making enormous contributions to research and producing cutting-edge technology, and its future is bright.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0600100)the National Key R&D Program of China (2020YFA0406100)+1 种基金the National Natural Science Foundation of China (21925206)National Natural Science Foundation of China (22332005)
文摘Development of non-noble-metal electrocatalysts with robust oxygen evolution reaction(OER)at the industrially required current density is desirable but still lacking for promising industrial-scale water electrolysis.Here,we report one cobalt phosphide-based heterostructure anode(denoted as Co_(x)P-HS hereafter)to exhibit extremely robust alkaline OER at 500 mA cm^(−2).Together with home-made NiMoOx cathode,we could fabricate one efficient two-electrode overall water splitting system,based on which one photovoltaic-driven electrochemical(PV-EC)water splitting device was further constructed for robust solar-to-hydrogen(STH)conversion with efficiency of over∼27.10%under one sun illumination.The extraordinary OER stability of our catalyst was unraveled to predominantly result from all-for-one design of multiple structural parameters,where the quasi-in situ growth of catalyst is favorable to prevent physical exfoliation of catalyst,while the local structure featured with two-dimensional morphology,polymorphic heterostructure and sulfur-doping modulation is highly desirable for efficient charge transfer and surface catalysis,leading to excellent electrochemical stability.
基金supported by the National Natural Science Foundation of China(No.21975151)China Postdoctoral Science Foundation(No.2023M733452).
文摘Pt-rare-earth(PtRE)alloys are considered to be highly promising catalysts for oxygen reduction reaction(ORR)in acidic electrolytes.However,the wet-chemical synthesis of PtRE nanoalloys still faces significant challenges.The precise reaction mechanism for ORR of these catalysts is still unclear on significant aspects involving the rate-determining step and the nature of the ligand effect.Herein,we report a class of solvothermal synthesis of PtRE(RE is Dy or La)nanoalloys.Such PtRE nanoalloys here are active and stable in acidic media,with both high mass activities enhanced by 2-5 times relative to commercial Pt/C catalyst and high stabilities indicative of the little activity decay and negligible structure change after 10,000 cycles.Density functional theory calculations firmly confirm that the ligand effect of RE elements accelerates an O-O bond scission and steers the rate-determining steps from OH^(*)+H^(+)+e-→H_(2)O(on pure Pt surface)to HOOH^(*)+H^(+)+e-→OH^(*)+H_(2)O(on the PtRE nanoalloy surface)for the fast reaction kinetics,which could be fine-tuned by regulating the RE electronic structures and consequently endows the maximal rate of ORR catalysis with PtDy alloy catalysts.
基金supported by Henan Province Key Research and Development and Promotion of Science and Technology Project(No.25A150001)the National Natural Science Foundation of China(Nos.22409171,22125303,92361302,and 92061203).
文摘Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined active sites and high loadings under precise control has become a hotly debated topic in scientific research.Metal-organic frameworks(MOFs),with their exceptional properties such as ultrahigh specific surface areas,precisely controllable structural de-signs,and highly flexible functional cus-tomization capabilities,are regarded as one of the ideal matrices for supporting and sta-bilizing SACs.This review provides an in-sightful overview of the diverse preparation strategies for MOFs-derived SACs.It comprehen-sively analyzes the unique advantages and challenges of each method in achieving efficient synthesis of SACs,emphasizing the crucial role of optimized processes in unlocking the antici-pated performance of SACs.Furthermore,this review delves into a series of advanced charac-terization techniques,including aberration-corrected scanning transmission electron mi-croscopy(AC-STEM),electron energy loss spectroscopy(EELS),X-ray absorption spec-troscopy(XAS),and infrared absorption spectroscopy(IRAS),offering valuable insights into the atomic-scale fine structures and properties of SACs,significantly advancing the under-standing of SAC mechanisms.Moreover,this review focuses on exploring the potential appli-cations of MOFs-derived SACs in electrocatalysis frontier fields.This comprehensive exami-nation lays a solid theoretical foundation and provides a directional guidance for the rational design and controllable synthesis of high-performance MOFs-derived SACs.
基金National Key R&D Program of China (2023YFA1508001 and 2023YFA1508002)National Natural Science Foundation of China (22272120 and U2202251)+1 种基金Hainan Province Science and Technology Special Fund(ZDYF2023SHFZ120)Research Foundation of Marine Science and Technology Collaborative Innovation Center of Hainan University (XTCX2022HYB01)。
文摘Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.
文摘In fulfillment of the national science-and-technology development agenda, the Department of Chemical Sciences of the National Natural Science Foundation of China (NSFC) convened the Strategic Symposium on the Fifteenth FiveYear (20262030) Development Plan for Electrochemistry held in Xiamen on 29 August, 2025-the culminating year of the Fourteenth Five-Year (2021-2025) Development Plan. More than forty leading experts in the field of electrochemistry participated with spanning nine thematic fronts: Interfacial Electrocatalysis, Interfacial Electrochemistry for Energy Storage, Bioelectrochemistry, Electrochemistry of Hydrogen Energy, Electrochemical Micro-/Nano-Manufacturing, Operando Electrochemical Characterization, Electro-Thermal Coupling Catalysis, Theoretical and Computational Electrochemistry,and Electrochemical Synthesis. The forum assembled China's foremost electrochemical expertise to blueprint high-quality disciplinary growth for the coming five-year period, thereby serving overarching national strategic needs and sharpening the international competitiveness of Chinese electrochemistry.This paper is presented to highlight the strategic needs and priority areas for the next five years (2026-2030) based on this symposium. The development status of basic research and applied basic research in China's electrochemistry field is systematically reviewed. The in-depth analyses of the existing problems and key challenges in the research and development of electrochemistry related fields are outlined, and the frontier research areas and development trends in the next 5-10 years by integrating national major strategic needs are discussed, which will further promote the academic community to reach a clearer consensus. The proposed strategic roadmap is intended to accelerate a sharpened community consensus, propel the discipline toward high-quality advancement, and furnish a critical reference for building China into a world-leading science and technology power.
基金supported by the National Natural Science Foundation of China(Projects 21790331,21603218,21703236 and 21872138)the Strategic Priority Research Program of the Chinese Academy of Sciences(Nos.XDB17020300 and XDA21030400)+1 种基金the Youth Innovation Promotion Association,CAS(2018219)DICP ZZBS201811
文摘In response to the awareness of limited fossil resources and environmental concerns,catalytic conversion of renewable lignocellulose biomass to value-added chemicals and fuels is of great significance and attractive for sustainable chemistry.Division of Biomass Conversion and Bio-Energy attached to Dalian National Laboratory for Clean Energy has devoted themselves to valorization of lignocellulose biomass since launched in 2011.Our research interests focus on breeding of biomass resources(inulin and microalgae),exploration of catalytic and biological technologies,and production of energy chemicals and fuels.Although lignocellulose biomass is renewable and abundant,the way of utilization should be reasonable according to its structural characteristics in view of efficiency and economy.In this review,to celebrate the DICP's 70 th anniversary,we will highlight the major fundamental advances in DICP about the conversion of lignocellulose to value-added chemicals and liquid fuels.Particular attention will be paid to the transformation of cellulose and its derivatives to glycols,acids and nitrogen-containing chemicals,hemicellulose-derived platform molecule furfural to jet fuels and lignin to aromatics using catalytic technologies.
文摘Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy.Precise synthesis of catalytically active nanostructures is one of the key challenges that hinder the practical application of many important energy‐related electrocatalytic reactions.Compared with conventional wet‐chemical,solid‐state and vapor deposition synthesis,electrochemical synthesis is a simple,fast,cost‐effective and precisely controllable method for the preparation of highly efficient catalytic materials.In this review,we summarize recent progress in the electrochemical synthesis of catalytic materials such as single atoms,spherical and shaped nanoparticles,nanosheets,nanowires,core‐shell nanostructures,layered nanomaterials,dendritic nanostructures,hierarchically porous nanostructures as well as composite nanostructures.Fundamental aspects of electrochemical synthesis and several main electrochemical synthesis methods are discussed.Structure‐performance correlations between electrochemically synthesized catalysts and their unique electrocatalytic properties are exemplified using selected examples.We offer the reader with a basic guide to the synthesis of highly efficient catalysts using electrochemical methods,and we propose some research challenges and future opportunities in this field.
基金supported by the National Natural Science Foundation of China (No.20877011)the DAAD (German Academic Exchange Service) Scientific Research Visiting Scholarship+3 种基金the Chinese National Programs for High Technology Research and Development (No.2011AA060604)the State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences (No.KF2009-17)the Key Laboratory of Industrial Ecology and Environmental Engineering,Ministry of Education of China (No.0802)the Scientific Research Foundation for Returned Overseas Chinese Scholars,Ministry of Education of China
文摘The concentration of polychlorinated biphenyls （PCBs） in the urban air of Dalian, China was monitored from November 2009 to October 2010 with active high-volume sampler and semipermeable membrane device （SPMD） passive sampler. The concentration of PCBs （particle ＋ gas） （∑PCBs） ranged from 18.6 to 91.0 pg/m3, with an average of 50.9 pg/m3, and the most abundant dioxin-like PCB （DL-PCBs） was PCB118. The WHO-TEQ values of DL-PCBs were 3.6--22.1 fg/m3, with an average of 8.5 fg/m3, and PCB126 was the maximum contributor to ZTEQ. There was a much larger amount of PCBs in the gas phase than in the particulate phase. The dominant PCB components were lower and middle molecular weight PCBs. With increasing chlorination level, the concentration of the PCB congeners in the air decreased. The gas-particulate partitioning of PCBs was different for the four seasons. The gas- particulate partitioning coefficients （logKp） vs. subcooled liquid vapor pressures （logPL~） of PCBs had reasonable correlations for different sampling sites and seasons. The absorption mechanism contributed more to the gas-particulate partitioning process than adsorption. Correlation analysis of meteorological parameters with the concentration of PCBs was conducted using SPSS packages. The ambient temperature and atmospheric pressure were important factors influencing the concentration of PCBs in the air. The distribution pattern of the congeners of PCBs and the dominant contributors to DL-PCBs and TEQ in active samples and SPMDs passive samples were similar. SPMD mainly sequestrated gas phase PCBs.
基金supported by the National Key R&D Program of China (2016YFB0600902)the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17000000)+2 种基金Dalian National Laboratory for Clean Energy (DNL180401)the Youth Innovation Promotion Association CASthe Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1: RG9/17, RG115/17, RG115/18 and Tier 2: MOE2016-T2-2-004
文摘Electrochemical CO2 reduction to chemicals or fuels presents one of the most promising strategies for managing the global carbon balance, which yet poses a significant challenge due to lack of efficient and durable electrocatalyst as well as the understanding of the CO2 reduction reaction(CO2RR) mechanism.Benefiting from the large surface area, high electrical conductivity, and tunable structure, carbon-based metal-free materials(CMs) have been extensively studied as cost-effective electrocatalysts for CO2RR.The development of CMs with low cost, high activity and durability for CO2RR has been considered as one of the most active and competitive directions in electrochemistry and material science.In this review article,some up-to-date strategies in improving the CO2RR performance on CMs are summarized.Specifically, the approaches to optimize the adsorption of CO2RR intermediates, such as tuning the physical and electronic structure are introduced, which can enhance the electrocatalytic activity of CMs effectively.Finally, some design strategies are proposed to prepare CMs with high activity and selectivity for CO2RR.
基金supported by the National Natural Science Foundation of China (No. 21577009)
文摘The concentration of short-chain polychlorinated paraffins(SCCPs) in the urban air of Dalian,China was monitored from September 2016 to August 2017 with a self-developed passive sampler(PAS1) and an active high-volume sampler, simultaneously. PAS1 successfully collected the entire target SCCPs in the ambient air. Air SCCPs sampled by PAS1 were found be in the linear uptake stage during 181 days of sampling. Passive and active samples showed comparable congener profiles, and the dominant contributors of SCCPs in the two kinds of samples were similar. A significant linear correlation was observed between the total concentration of SCCPs sampled by PAS1 and active sampler in the four seasons. The passive sampling rates of the PAS1 for the gas and particulate phases of SCCPs were measured. The quantitative structure–property relationship of the sampling rate of PAS1(Rair) for gas-phase SCCPs was studied. From the molecular point of view, Rairwas mainly affected by the molecular weight and sub-cooled liquid vapor pressure of SCCPs. In general, SCCPs in the urban air of Dalian mainly existed in gas phase,lower molecular weight SCCPs primarily occurred in the gas phase, whereas higher molecular weight SCCPs were predominately adsorbed or absorbed on airborne particles. The air concentration of SCCPs in the four seasons were different, the correlation of the concentration of SCCPs in the air with the meteorology parameters was conducted. The exposure risk by intake air SCCPs of the residents around the sampling sites was evaluated according to the European risk assessment standards.
基金the financial support from the National Natural Science Foundation of China(91545202)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB17020400)
文摘The effort on electrochemical reduction of COto useful chemicals using the renewable energy to drive the process is growing fast recently. In this review, we introduce the recent progresses on the electrochemical reduction of COin solid oxide electrolysis cells（SOECs）. At high temperature, only CO is produced with high current densities and Faradic efficiency while the reactor is complicated and a better sealing technique is urgently needed. The typical electrolytes such as zirconia-based oxides, ceria-based oxides and lanthanum gallates-based oxides, anodes and cathodes are introduced in this review, and the cathode materials, such as conventional metal–ceramics（cermets）, mixed ionic and electronic conductors（MIECs） are discussed in detail. In the future, to gain more value-added products, the electrolyte, cathode and anode materials should be developed to allow SOECs to be operated at temperature range of 573–873 K. At those temperatures, SOECs may combine the advantages of the low temperature system and the high temperature system to produce various products with high current densities.
文摘In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.
基金Financial support was provided by the Chinese Academy of Sciences–The World Academy of Sciences(CAS-TWAS)president fellowship。
文摘The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this field,the reported catalysts rarely deviate from the traditionally supported metal nanoparticle morphology,with the most simplistic method of enhancement being the addition of more metals to an already complex composition.Encapsulated catalysts,especially yolk@shell catalysts with hollow voids,offer answers to the most prominent issues faced by this field,coking and sintering,and further potential for more advanced phenomena,for example,the confinement effect,to promote selectivity or offer greater protection against coking and sintering.This work serves to demonstrate the current position of catalyst development in the fields of thermal CO_(2) reforming and hydrogenation,summarizing the most recent work available and most common metals used for these reactions,and how yolk@shell catalysts can offer superior performance and survivability in thermal CO_(2) reforming and hydrogenation to the more traditional structure.Furthermore,this work will briefly demonstrate the bespoke nature and highly variable yolk@shell structure.Moreover,this review aims to illuminate the spatial confinement effect and how it enhances yolk@shell structured nanoreactors is presented.
基金the Natural Science & Technology Foundation Council of Liaoning ProvinceOpen Laboratory of Carbon Resource Utilization of Da
文摘The methoxycarbonylations of cyclohexene and 1-decene with CO2 can take place under ambient conditions by catalysis of [Co]([Co]=Co(acac)(2), Co(OAc)(2), CoCl2) in the presence of ultraviolet irradiation.
文摘Copper-indium bimetallic catalysts with a dendritic structure are fabricated by a two-step electrodeposition method using a hydrogen evolution template for the CO2 electroreduction reaction(CO2RR).The dendritic Cu-In-30 catalyst electrodeposited for 30 min shows the highest specific surface area and exposes the most active sites,resulting in improved CO2RR activity.The dendritic Cu-In-30 catalyst exhibits distinctly higher formate partial current density(42.0 m A cm^-2)and Faradaic efficiency(87.4%)than those of the In-30 catalyst without the dendritic structure(the formate partial current density and Faradaic efficiency are 4.6 m A cm^-2 and 57.0%,respectively)at-0.85 V vs.reversible hydrogen electrode,ascribed to the increased specific surface area.The Cu-In-30 catalyst can maintain stable performance for 12 h during the CO2RR.In addition,the intrinsic current density of Cu-In-30 with the dendritic structure(4.8 m A cm^-2)is much higher than that of In-30 without the dendritic structure(2.1 m A cm^-2),indicating that the dendritic structure promotes the CO2RR,possibly due to additional coordination unsaturated atoms.
文摘The continuous wavelength chemical oxygen-iodine laser can be turned into pulse operation mode in order to obtain high energy and high pulse power. We propose an approach to produce iodine atoms instantaneously by pulsed gas discharge with the assistance of spark pre-ionization to achieve the pulsed goal. The influence of spark pre-ionization on discharge homogeneity is discussed. Voltage-current characteristics are shown and discussed in existence of the pre-ionization capacitor and peaking capacitor. The spark pre-ionization and peaking capacitor are very helpful in obtaining a stable and homogeneous discharge. The lasing is achieved at the total pressure of 2.2-2.9 kPa and single pulse energy is up to 180 mJ, the corresponding specific output energy is 1.0 3/L.
基金the frame of ERC Synergy SCOPE(project 810182)PRIN 2015 SMARTNESS project nr.2015K7FZLH projects which are gratefully acknowledgeda SINCHEM Grant.SINCHEM is a Joint Doctorate program selected under the Erasmus Mundus Action 1 Programme(FPA 2013-0037)。
文摘The direct electrocatalytic synthesis of ammonia from N2 and H2O by using renewable energy sources and ambient pressure/temperature operations is a breakthrough technology,which can reduce by over 90%the greenhouse gas emissions of this chemical and energy storage process.We report here an in-situ electrochemical activation method to prepare Fe2O3-CNT(iron oxide on carbon nanotubes)electrocatalysts for the direct ammonia synthesis from N2 and H2O.The in-situ electrochemical activation leads to a large increase of the ammonia formation rate and Faradaic efficiency which reach the surprising high values of 41.6μg mgcat^−1 h^−1 and 17%,respectively,for an in-situ activation of 3 h,among the highest values reported so far for non-precious metal catalysts that use a continuous-flow polymer-electrolytemembrane cell and gas-phase operations for the ammonia synthesis hemicell.The electrocatalyst was stable at least 12 h at the working conditions.Tests by switching N2 to Ar evidence that ammonia was formed from the gas-phase nitrogen.The analysis of the changes of reactivity and of the electrocatalyst characteristics as a function of the time of activation indicates a linear relationship between the ammonia formation rate and a specific XPS(X-ray-photoelectron spectroscopy)oxygen signal related to O2−in iron-oxide species.This results together with characterization data by TEM and XRD suggest that the iron species active in the direct and selective synthesis of ammonia is a maghemite-type iron oxide,and this transformation from the initial hematite is responsible for the in-situ enhancement of 3-4 times of the TOF(turnover frequency)and NH3 Faradaic efficiency.This transformation is likely related to the stabilization of the maghemite species at CNT defect sites,although for longer times of preactivation a sintering occurs with a loss of performances.
