Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is chall...Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.展开更多
TiB2/Al-30Si composites were fabricated via in-situ melt reaction under high-energy ultrasonic field. The microstructure and wear properties of the composite were investigated by XRD, SEM and dry sliding testing. The ...TiB2/Al-30Si composites were fabricated via in-situ melt reaction under high-energy ultrasonic field. The microstructure and wear properties of the composite were investigated by XRD, SEM and dry sliding testing. The results indicate that TiB2 reinforcement particles are uniformly distributed in the aluminum matrix under high-energy ultrasonic field. The morphology of the TiB2 particles is in circle-shape or quadrangle-shape, and the size of the particles is 0.1-1.5μm. The primary silicon particles are in quadrangle-shape and the average size of them is about 10μm. Hardness values of the Al-30Si matrix alloy and the TiB2/Al-30Si composites considerably increase as the high energy ultrasonic power increases. In particular, the maximum hardness value of the in-situ composites is about 1.3 times as high as that of the matrix alloy when the ultrasonic power is 1.2 kW, reaching 412 MPa. Meanwhile, the wear resistance of the in-situ TiB2/Al-30Si composites prepared under high-energy ultrasonic field is obviously improved and is insensitive to the applied loads of the dry sliding testing.展开更多
In-situ reactive compatibilization of high-density polyethylene (HDPE)/ground tire rubber (GTR) blends by dicumyl peroxide (DCP) and HY-2045 - a kind of thermoplastic phenolic resin without catalyst was inves...In-situ reactive compatibilization of high-density polyethylene (HDPE)/ground tire rubber (GTR) blends by dicumyl peroxide (DCP) and HY-2045 - a kind of thermoplastic phenolic resin without catalyst was investigated by studying the mor-phology, stress and strain behavior, dynamic mechanical properties and crystallization performance of the blends. Scanning e-lectron microscopy (SEM) results show that there are a lot of fibrous materials distributing in the interface, which connects the dispersed phase with the matrix and obtains better interfacial strength for prominent mechanical properties. The addition of compatibilizers results in the decrease of crystallinity of the blends and the disappearance of an obvious yield phenomenon, which was proved by the differential scanning calorimeter (DSC) test and X-ray diffraction (XRD) characterization Although the crystallinity of the blends decreases,the tensile strength and tensile strain of the blends significantly increases, especially for the HDPE/GTR/DCP/HY-2045 blends, which is possibly attributed to the good compatibility of the blends owing to the in-situ interface crosslinking. In addition, it is found that the compatibilizing HDPE/GTR blends shows a higher tan^ peak temperature and a broaden transition peak for GTR phase.展开更多
Objective: To investigate the changes of autonomic nervous system (ANS) function during the initial phase at acute high-altitude exposure. Methods: Ninety-nine healthy sea-level male residents were studied in Chengdu ...Objective: To investigate the changes of autonomic nervous system (ANS) function during the initial phase at acute high-altitude exposure. Methods: Ninety-nine healthy sea-level male residents were studied in Chengdu plain and then Tibet plateau. Heart rate variability (HRV), cold pressor test (CPT), resting heart rate (HR) and blood pressure (BP) were measured at baseline (560 m altitude) and in 2 to 4 d after arriving at Tibet plateau (3 675 m altitude) to assess the ANS function. Results: Compared with baseline, on day 2 in Tibet the standard deviation of normal to normal intervals (SDNN), high-frequency (HF) power, total power (TP), root mean square of delta RR (rMSSD), percentage of delta RR>50 ms (PNN50), normalized high-frequency (HFnu) and fractal dimension (FD) decreased significantly (SDNN, HF, TP P<0.01, rMSSD, PNN50, HFnu, FD P<0.05), while the normalized low-frequency (LFnu) and LF/HF increased significantly (P<0.01). During day 3–4 in Tibet, SDNN, rMSSD, HF, TP and HFnu tended to rebound while LFnu and LF/HF decreased towards baseline day by day. In addition, in Tibet the increase in systolic pressure (SP) and diastolic pressure (DP) during CPT decreased significantly (P<0.01, 0.05), but resting HR increased compared with baseline (P<0.01). Conclusion: ANS modulation is generally blunted, and the relatively predominant sympathetic control is enhanced originally, then it reverts to the sea level states gradually during the initial days of acute high-altitude exposure.展开更多
The wetlands on the Zoige Plateau have experienced serious degradation,with most of the original marsh being converted to marsh meadow or meadow.Based on the 3 wetland degradation stages,we determined the effects of w...The wetlands on the Zoige Plateau have experienced serious degradation,with most of the original marsh being converted to marsh meadow or meadow.Based on the 3 wetland degradation stages,we determined the effects of wetland degradation on the structure and relative abundance of nitrogencycling(nitrogen-fixing,ammonia-oxidizing,and denitrifying) microbial communities in 3 soil types(intact wetland:marsh soil;early degrading wetland:marsh meadow soil;and degraded wetland:meadow soil) using 454-pyrosequencing.The structure and relative abundance of nitrogen-cycling microbial communities differed in the 3 soil types.Proteobacteria was the predominant phylum in most soil samples but the most abundant soil nitrogenfixing and denitrifying microbial bacteria differed at the class,order,family,and genus levels among the 3soil types.At the genus level,the majority of nitrogenfixing bacterium sequences related to Bradyrhizobium were from marsh and marsh meadow soils;whereas those related to Geobacter originated from meadow soil.The majority of ammonia-oxidizing bacterium sequences related to Nitrosospira were from marsh(except for the 40-60 cm layer),marsh meadow and meadow soils;whereas those related to Candidatus Solibacter originated from 40-60 cm layer of marsh soil.The majority of denitrifying bacterium sequences related to Candidatus Solibacter and Anaeromyxobacter were from marsh and meadow soils;whereas those related to Herbaspirillum originated from meadow soil.The distribution of operational taxonomic units(OTUs)and species were correlated with soil type based upon Venn and Principal Coordinates Analysis(PCoA).Changes in soil type,caused by different water regimes were the most important factors influencing compositional changes in the nitrogen-fixing,ammonia-oxidizing,and denitrifying microbial communities.展开更多
Exploring non‐precious metal catalysts for the oxygen reduction reaction (ORR) is essential for fuel cells and metal–air batteries. Herein, we report a Fe‐N‐C catalyst possessing a high specific surface area (1...Exploring non‐precious metal catalysts for the oxygen reduction reaction (ORR) is essential for fuel cells and metal–air batteries. Herein, we report a Fe‐N‐C catalyst possessing a high specific surface area (1501 m2/g) and uniformly dispersed iron within a carbon matrix prepared via a two‐step pyrolysis process. The Fe‐N‐C catalyst exhibits excellent ORR activity in 0.1 mol/L NaOH electrolyte (onset potential, Eo=1.08 V and half wave potential, E1/2=0.88 V vs. reversible hydrogen electrode) and 0.1 mol/L HClO4 electrolyte (Eo=0.85 V and E1/2=0.75 V vs. reversible hydrogen electrode). The direct methanol fuel cells employing Fe‐N‐C as the cathodic catalyst displayed promising per‐formance with a maximum power density of 33 mW/cm2 in alkaline media and 47 mW/cm2 in acidic media. The detailed investigation on the composition–structure–performance relationship by X‐ray diffraction, X‐ray photoelectron spectroscopy and Mo-ssbauer spectroscopy suggests that Fe‐N4, together with graphitic‐N and pyridinic‐N are the active ORR components. The promising direct methanol fuel cell performance displayed by the Fe‐N‐C catalyst is related to the intrinsic high catalytic activity, and critically for this application, to the high methanol tolerance.展开更多
Combustion synthesis involving metallothermic reduction of Fe2O3 and TiO2 was conducted in the mode of self-propagating high-temperature synthesis(SHS)to fabricate FeAl-based composites with dual ceramic phases,TiB2/A...Combustion synthesis involving metallothermic reduction of Fe2O3 and TiO2 was conducted in the mode of self-propagating high-temperature synthesis(SHS)to fabricate FeAl-based composites with dual ceramic phases,TiB2/Al2O3 and TiC/Al2O3.The reactant mixture included thermite reagents of 0.6Fe2O3+0.6TiO2+2Al,and elemental Fe,Al,boron,and carbon powders.The formation of xFeAl−0.6TiB2−Al2O3 composites with x=2.0−3.6 and yFeAl−0.6TiC−Al2O3 composites with y=1.8−2.75 was studied.The increase of FeAl causes a decrease in the reaction exothermicity,thus resulting in the existence of flammability limits of x=3.6 and y=2.75 for the SHS reactions.Based on combustion wave kinetics,the activation energies of Ea=97.1 and 101.1 kJ/mol are deduced for the metallothermic SHS reactions.XRD analyses confirm in situ formation of FeAl/TiB2/Al2O3 and FeAl/TiC/Al2O3 composites.SEM micrographs exhibit that FeAl is formed with a dense polycrystalline structure,and the ceramic phases,TiB2,TiC,and Al2O3,are micro-sized discrete particles.The synthesized FeAl−TiB2−Al2O3 and FeAl−TiC−Al2O3 composites exhibit the hardness ranging from 12.8 to 16.6 GPa and fracture toughness from 7.93 to 9.84 MPa·m1/2.展开更多
Iron-based single-atom catalysts with nitrogen-doped carbon as support(Fe-SA/NPC)are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells.However,synthesizing high-loadin...Iron-based single-atom catalysts with nitrogen-doped carbon as support(Fe-SA/NPC)are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells.However,synthesizing high-loading Fe-SA catalysts by a simple procedure remains challenging.Herein,we report a high-loading(7.5 wt%)Fe-SA/NPC catalyst prepared by carbon-assisted pyrolysis of metal complexes.Both the nitrogen-doped porous carbon(NPC)support with high specific surface area and ο-phenylenediamine(o-PD)play key roles role in the preparation of high-loading Fe-SA/NPC catalysts.The results of X-ray photoelectron spectroscopy,high-angle annular dark-field scanning transmission electron microscopy,and X-ray absorption fine structure spectroscopy experiments show that the Fe atoms are anchored on the carbon carriers in a single-atom site configuration and coordinated with four of the doped nitrogen atoms of the carbon substrates(Fe-N_(4)).The activities of the Fe-SA/NPC catalysts in the oxygen reduction reaction increased with increasing iron loading.The optimized 250Fe-SA/NPC-800 catalyst exhibited an onset potential 0.97 V of and a half-wave potential of 0.85 V.Our study provides a simple approach for the large-scale synthesis of high-loading single-atom catalysts.展开更多
The mechanism of idiopathic ventricular tachycardia originating from the right ventricular outflow tract (RVOT) is not clear. Many clinical reports have suggested a mechanism of triggered activity. However, there ar...The mechanism of idiopathic ventricular tachycardia originating from the right ventricular outflow tract (RVOT) is not clear. Many clinical reports have suggested a mechanism of triggered activity. However, there are few studies investigating this be- cause of the technical difficulties associated with examining this theory. The L-type calcium current (/Ca-L), an important in- ward current of the action potential (AP), plays an important role in arrhythmogenesis. The aim of this study was to explore differences in the APs of right ventricular (RV) and RVOT cardiomyocytes, and differences in electrophysiological character- istics of the ICa-L in these myocytes. Rabbit RVOT and RV myocytes were isolated and their AP and Ic,-L were investigated us- ing the patch-clamp technique. RVOT cardiomyocytes had a wider range of AP duration (APD) than RV cardiomyocytes, with some markedly prolonged APDs and markedly shortened APDs. The markedly shortened APDs in RVOT myocytes were abolished by treatment with 4-AP, an inhibitor of the transient outward potassium current, but the markedly prolonged APDs remained, with some myocytes with a long AP plateau not repolarizing to resting potential. In addition, early afterdepolariza- tion (EAD) and second plateau responses were seen in RVOT myocytes but not in RV myocytes. RVOT myocytes had a high- er current density for/Ca-L than RV myocytes (RVOT (13.16±0.87) pA pF-1, RV (8.59±1.97) pA pF-1; P〈0.05). The ICa-L and the prolonged APD were reduced, and the EAD and second plateau response disappeared, after treatment with nifedipine (10 μmol L^-1), which blocks the Ica-L. In conclusion, there was a wider range of APDs in RVOT myocytes than in RV myocytes, which is one of the basic factors involved in arrhythmogenesis. The higher current density for ICa-L is one of the factors causing prolongation of the APD in RVOT myocytes. The combination of EAD with prolonged APD may be one of the mechanisms of RVOT-VT generation.展开更多
Deforestation to reclaim land often triggers severe soil erosion in the Guizhou Karst Plateau. 137Cs dating of the deposited sediments in the karst depression bottom was used to estimate soil losses by surface erosion...Deforestation to reclaim land often triggers severe soil erosion in the Guizhou Karst Plateau. 137Cs dating of the deposited sediments in the karst depression bottom was used to estimate soil losses by surface erosion since deforestation started in 1979 on hillslopes in the Shirenzhai catchment, Puding County, Guizhou Province. The catchment has a drainage area of 0.054 km2. The average 137Cs contents of the top and peak layers in five cores of the depression bottom (with an area of 2652 m2), collected in 2009, were 2.35 and 7.25 Bq kg-1, respectively. The medium depths in the depression (which ranged between 84 cm and 113.5 cm with a mean value of 92.1 cm) showed the presence of sediments deposited in 1979. The total volume and weight of the deposited sediments since 1979 were estimated to be 1965 m3 and 2496 t, respectively. The depression bottom can be treated as a temporary impoundment and its sediment trapping efficiency was estimated to be 0.7. The relevant average soil erosion rate on the hillslopes was 2315 t km-2 yr-1 since 1979. The mean 137Cs inventory of the five cores was 7693 Bq m-2, which was ~10 times the local reference inventory of 782 Bq m-2. The total 137Cs activity of the sediments in the bottom was 20.4×106 Bq, and the relevant 137Cs inventory loss from the hillslopes was 358 Bq m-2 (since 1954), which accounted for 45.8% of the reference inventory. As soil erosion was not severe before and after the period of deforestation and following cultivation in 1979-1990, the erosion rates on the hillslopes could potentially reach 7000 t km-2 yr-1.展开更多
A PtFe/C catalyst has been synthesized by impregnation and high-temperature reduction followed by acid-leaching. X-ray diffraction, X-ray photoelectron spectroscopy and X-ray atomic near edge spectroscopy characteriza...A PtFe/C catalyst has been synthesized by impregnation and high-temperature reduction followed by acid-leaching. X-ray diffraction, X-ray photoelectron spectroscopy and X-ray atomic near edge spectroscopy characterization reveal that PtgFe alloy formation occurs during high-temperature reduction and that unstable Fe species are dissolved into acid solution. The difference in Fe concentration from the core region to the surface and strong O-Fe bonding may drive the outward diffusion of Fe to the highly corrugated Pt-skeleton, and the resulting highly dispersed surface FeOx is stable in acidic medium, leading to the construction of a PtBFe@Pt-FeOx architecture. The as prepared PtFe/C catalyst demonstrates a higher activity and comparable durability for the oxygen reduction reaction compared with a Pt/C catalyst, which might be due to the synergetic effect of surface and subsurface Fe species in the PtFe/C catalyst.展开更多
Developing low-cost, high-performance elec- trocatalysts for the oxygen reduction reaction (ORR) is crucial for implementation of fuel cells and metal-air batteries into practical applications. Graphene-based cataly...Developing low-cost, high-performance elec- trocatalysts for the oxygen reduction reaction (ORR) is crucial for implementation of fuel cells and metal-air batteries into practical applications. Graphene-based catalysts have been extensively investigated for ORR in alkaline electrolytes. However, their performance in acidic electrolytes still requires further improvement compared to the Pt/C catalyst. Here we report a self-templating approach to prepare graphene-based sandwich-like porous carbon nanosheets for efficient ORR in both alkaline and acidic electrolytes. Graphene oxides were first used to adsorb m-phenylenediamine molecules which can form a nitrogen-rich polymer network after oxidative poly- merization. Then iron (Fe) salt was introduced into the polymer network and transformed into ORR active Fe-N-C sites along with Fe, FeS, and FEN0.05 nanopartides after pyr- olysis, generating ORR active sandwich-like carbon na- nosheets. Due to the presence of multiple ORR active sites. The as-obtained catalyst exhibited prominent ORR activity with a half-wave potential -30 mV more positive than Pt/C in 0.1 mol L-1 KOH, while the half-wave potential of the catalyst was only -40 mV lower than that of commercial Pt/C in 0.1 mol L-1 HClO4. The unique planar sandwich-like structure could expose abundant active sites for ORR. Meanwhile, the graphene layer and porous structure could simultaneously enhance electrical conductivity and facilitate mass transport. The prominent electrocatalytic activity and durability in both alkaline and acidic electrolytes indicate that these carbon na- nosheets hold great potential as alternatives to precious metal- based catalysts, as demonstrated in zinc-air batteries and proton exchange membrane fuel cells.展开更多
In energy industries, it is always of difficulty to produce high heat value(HHV) gas continuously using pulverized coal. In this paper, a new type furnace for partitioned alternative gasification using pulverized co...In energy industries, it is always of difficulty to produce high heat value(HHV) gas continuously using pulverized coal. In this paper, a new type furnace for partitioned alternative gasification using pulverized coal is developed, in which the oxidation and reduction reaction occur alternatively with the dropping of pulverized coal and finally HHV gas could be continuously obtained at the reduction zone exit and low heat value(LHV) gas at the oxidation zone exit. Furthermore, the gasification characteristics and their factors in furnace are numerically simulated under two dimensional model with a self-coded program, based on heat, mass and energy transfer as well as reaction principles. It is found that the producing rate of HHV gas is 1.10Nm3/kg with heat value of ll.72MJ/Nm3, how- ever, that of LHV gas is 2.58Nm3/kg with heat value of 5.30MJ/Nm3, and the coal gas efficiency is 81.16% under optimized conditions.展开更多
Cobalt-based oxygenic compounds Co(OH)2,CoO and Co3 O4 are attractive for electrochemical energy storage owing to their high theoretical capacities and pseudocapacitive properties.Despite the great efforts to their co...Cobalt-based oxygenic compounds Co(OH)2,CoO and Co3 O4 are attractive for electrochemical energy storage owing to their high theoretical capacities and pseudocapacitive properties.Despite the great efforts to their compositional and morphological regulations,the performances to date are still quite limited owing to the low active surface area and sluggish charge transfer kinetics.Herein,different Co-based nanocrystals(Co-NCs)were conveniently anchored on the hierarchical nitrogen-doped carbon nanocages(hNCNCs)with high specific surface area and coexisting micro-meso-macropores to decrease the size and facilitate the charge transfer.Accordingly,a high specific capacity of1170 Fg^-1 is achieved at 2 Ag^-1 for the Co(OH)2/hNCNCs hybrid,in which the capacitance of Co(OH)2(2214 F gco(OH)2)is approaching to its theoretical maximum(2595 Fg^-1),demonstrating the high utilization of active materials by the hybridization with N-doped nanocarbons.This study also reveals that these Co-NCs store/release electrical energy via the same reversible redox reaction despite their different pristine compositions.This insight on the energy storage of Co-based nanomaterials suggests that the commonly-employed transformation of the Co-NCs from Co(OH)2 to CoO and Co3 O4 on carbon supports is unnecessary and even could be harmful to the energy storage performance.The result is instructive to develop high-energy-density electrodes from transition metal compounds.展开更多
The rechargeable aluminum-sulfur(Al-S)battery is a promising alternative-energy storage device with high energy density and made of cheap raw materials.However,Al-S batteries face several obstacles,especially the shut...The rechargeable aluminum-sulfur(Al-S)battery is a promising alternative-energy storage device with high energy density and made of cheap raw materials.However,Al-S batteries face several obstacles,especially the shuttle effect.Herein,a binder-free S@Ti_(3)C_(2)T_(x)sandwich structure film with uniform sulfur dispersion was designed.The two-dimensional(2D)layered material Ti_(3)C_(2)T_(x) not only has the function of binder and conductive agent but also is a promising host for sulfur anchoring.As a result,S@Ti_(3)C_(2)T_(x)film showed an initial capacity of 489 mA h g^(−1)at 300 mA g^(−1) and retained the value at 415 mA h g^(−1)after 280 stable cycles,with an average Coulombic efficiency of~95%.The film displayed higher capacity and stability than the S+Ti_(3)C_(2)T_(x)cathode prepared by the slurry-coating method(the initial capacity was 317 mA h g^(−1)and then decayed to 222 mA h g^(−1) after 160 cycles).The main capacity of S@Ti_(3)C_(2)T_(x) film in the Al-S battery came from the reversible redox reaction of S^(2−) and S.This new 2D material combined with a controllable electrode structure design paves the way for the development of Al-S batteries.展开更多
Hierarchical TiO2 photocatalysts with a one-dimensional heterojunction were synthesized via a facile template-free hydrothermal method. The TiO2 photo- catalysts were flower-like microspheres with a 3 μm diameter. Th...Hierarchical TiO2 photocatalysts with a one-dimensional heterojunction were synthesized via a facile template-free hydrothermal method. The TiO2 photo- catalysts were flower-like microspheres with a 3 μm diameter. The base structure of the flower-like microspheres was a uniform nanowire with a 10 nm diameter. Anatase films were evenly coated onto the surface of the rutile TiO2 nanowires to form a one-dimensional core--shell base structure. This kind of one-dimensional heterojunction is conducive to the separation of charge carriers. In addition, the hierarchical TiO2 microspheres possessed a good mesoporous structure with a high specific surface area of 260 m2/g. Thus, the light scattering and utilization efficiency were improved in this structure. The photocatalysts exhibited better performance in both photocatalytic oxidation and reduction reactions. Moreover, the novel TiO2 photocatalysts displayed excellent stability in these reactions. This kind of hierarchical TiO2 structure has never been reported in the literature. The hierarchical structure and one-dimensional heterojunction were vital to the increase in quantum efficiency. Therefore, these hierarchical TiO2 photocatalysts have potential applications in the environmental and energy fields, such as in photocatalytic degradation, hydrogen production, Li-ion batteries, and dye-sensitized solar cells.展开更多
Designing highly selective and efficient singleatom electrocatalysts is essential for ammonia production under ambient conditions. This paper describes a density functional theory study on exploring the performance tr...Designing highly selective and efficient singleatom electrocatalysts is essential for ammonia production under ambient conditions. This paper describes a density functional theory study on exploring the performance trends of transition metal complexes with P-based ligands in nitrogen reduction reaction(NRR) and further develops a design principle for high-performance single-atom catalysts(SACs)of NRR. Among the explored catalysts, W@BP(0.40 eV),Ta@BP(0.47 eV), and Nb@BP(0.53 eV) are identified as remarkable candidates with low free energy change in the potential-limiting step, high stability and high electrical conductivity for NRR. It is worth noting that almost all SACs with P-based ligands exhibit high NRR selectivity, due to the fact that they adsorb *N_(2) more strongly than *H. The adsorption free energy of *N_(2) H can be considered as a descriptor for the intrinsic activity trends in NRR. Furthermore, by constructing a volcano plot of the activity against the electronic charge on metal centers, it is demonstrated that the metal center with a moderate amount of positive charge can promote the catalytic performance of NRR.展开更多
文摘Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.
基金Project(51174098)supported by the National Natural Science Foundation of ChinaProject(kjsmcx0903)supported by the Foundation of the Jiangsu Province Key Laboratory of Materials Tribology,China+2 种基金Project(1202015B)supported by the Postdoctoral Science Foundation of Jiangsu Province,ChinaProject(03)supported by the Undergraduate Practice-Innovation Training Foundation of Jiangsu University,ChinaProjects(GY2012020,GY2013032)supported by the Science and Technology Support Plan Project Foundation of Zhenjiang City,China
文摘TiB2/Al-30Si composites were fabricated via in-situ melt reaction under high-energy ultrasonic field. The microstructure and wear properties of the composite were investigated by XRD, SEM and dry sliding testing. The results indicate that TiB2 reinforcement particles are uniformly distributed in the aluminum matrix under high-energy ultrasonic field. The morphology of the TiB2 particles is in circle-shape or quadrangle-shape, and the size of the particles is 0.1-1.5μm. The primary silicon particles are in quadrangle-shape and the average size of them is about 10μm. Hardness values of the Al-30Si matrix alloy and the TiB2/Al-30Si composites considerably increase as the high energy ultrasonic power increases. In particular, the maximum hardness value of the in-situ composites is about 1.3 times as high as that of the matrix alloy when the ultrasonic power is 1.2 kW, reaching 412 MPa. Meanwhile, the wear resistance of the in-situ TiB2/Al-30Si composites prepared under high-energy ultrasonic field is obviously improved and is insensitive to the applied loads of the dry sliding testing.
文摘In-situ reactive compatibilization of high-density polyethylene (HDPE)/ground tire rubber (GTR) blends by dicumyl peroxide (DCP) and HY-2045 - a kind of thermoplastic phenolic resin without catalyst was investigated by studying the mor-phology, stress and strain behavior, dynamic mechanical properties and crystallization performance of the blends. Scanning e-lectron microscopy (SEM) results show that there are a lot of fibrous materials distributing in the interface, which connects the dispersed phase with the matrix and obtains better interfacial strength for prominent mechanical properties. The addition of compatibilizers results in the decrease of crystallinity of the blends and the disappearance of an obvious yield phenomenon, which was proved by the differential scanning calorimeter (DSC) test and X-ray diffraction (XRD) characterization Although the crystallinity of the blends decreases,the tensile strength and tensile strain of the blends significantly increases, especially for the HDPE/GTR/DCP/HY-2045 blends, which is possibly attributed to the good compatibility of the blends owing to the in-situ interface crosslinking. In addition, it is found that the compatibilizing HDPE/GTR blends shows a higher tan^ peak temperature and a broaden transition peak for GTR phase.
文摘Objective: To investigate the changes of autonomic nervous system (ANS) function during the initial phase at acute high-altitude exposure. Methods: Ninety-nine healthy sea-level male residents were studied in Chengdu plain and then Tibet plateau. Heart rate variability (HRV), cold pressor test (CPT), resting heart rate (HR) and blood pressure (BP) were measured at baseline (560 m altitude) and in 2 to 4 d after arriving at Tibet plateau (3 675 m altitude) to assess the ANS function. Results: Compared with baseline, on day 2 in Tibet the standard deviation of normal to normal intervals (SDNN), high-frequency (HF) power, total power (TP), root mean square of delta RR (rMSSD), percentage of delta RR>50 ms (PNN50), normalized high-frequency (HFnu) and fractal dimension (FD) decreased significantly (SDNN, HF, TP P<0.01, rMSSD, PNN50, HFnu, FD P<0.05), while the normalized low-frequency (LFnu) and LF/HF increased significantly (P<0.01). During day 3–4 in Tibet, SDNN, rMSSD, HF, TP and HFnu tended to rebound while LFnu and LF/HF decreased towards baseline day by day. In addition, in Tibet the increase in systolic pressure (SP) and diastolic pressure (DP) during CPT decreased significantly (P<0.01, 0.05), but resting HR increased compared with baseline (P<0.01). Conclusion: ANS modulation is generally blunted, and the relatively predominant sympathetic control is enhanced originally, then it reverts to the sea level states gradually during the initial days of acute high-altitude exposure.
基金financially supported by the 11th Five Years Key Programs for Science and Technology Development of China (Grant No.2007BAC18B03)
文摘The wetlands on the Zoige Plateau have experienced serious degradation,with most of the original marsh being converted to marsh meadow or meadow.Based on the 3 wetland degradation stages,we determined the effects of wetland degradation on the structure and relative abundance of nitrogencycling(nitrogen-fixing,ammonia-oxidizing,and denitrifying) microbial communities in 3 soil types(intact wetland:marsh soil;early degrading wetland:marsh meadow soil;and degraded wetland:meadow soil) using 454-pyrosequencing.The structure and relative abundance of nitrogen-cycling microbial communities differed in the 3 soil types.Proteobacteria was the predominant phylum in most soil samples but the most abundant soil nitrogenfixing and denitrifying microbial bacteria differed at the class,order,family,and genus levels among the 3soil types.At the genus level,the majority of nitrogenfixing bacterium sequences related to Bradyrhizobium were from marsh and marsh meadow soils;whereas those related to Geobacter originated from meadow soil.The majority of ammonia-oxidizing bacterium sequences related to Nitrosospira were from marsh(except for the 40-60 cm layer),marsh meadow and meadow soils;whereas those related to Candidatus Solibacter originated from 40-60 cm layer of marsh soil.The majority of denitrifying bacterium sequences related to Candidatus Solibacter and Anaeromyxobacter were from marsh and meadow soils;whereas those related to Herbaspirillum originated from meadow soil.The distribution of operational taxonomic units(OTUs)and species were correlated with soil type based upon Venn and Principal Coordinates Analysis(PCoA).Changes in soil type,caused by different water regimes were the most important factors influencing compositional changes in the nitrogen-fixing,ammonia-oxidizing,and denitrifying microbial communities.
基金supported by the“Strategic Priority Research Program”of the Chinese Academy of Sciences(XDA09030104)the National Basic Research Program of China(973 Program,2012CB215500)+1 种基金the National Natural Science Foundation of China(2157625850823008)~~
文摘Exploring non‐precious metal catalysts for the oxygen reduction reaction (ORR) is essential for fuel cells and metal–air batteries. Herein, we report a Fe‐N‐C catalyst possessing a high specific surface area (1501 m2/g) and uniformly dispersed iron within a carbon matrix prepared via a two‐step pyrolysis process. The Fe‐N‐C catalyst exhibits excellent ORR activity in 0.1 mol/L NaOH electrolyte (onset potential, Eo=1.08 V and half wave potential, E1/2=0.88 V vs. reversible hydrogen electrode) and 0.1 mol/L HClO4 electrolyte (Eo=0.85 V and E1/2=0.75 V vs. reversible hydrogen electrode). The direct methanol fuel cells employing Fe‐N‐C as the cathodic catalyst displayed promising per‐formance with a maximum power density of 33 mW/cm2 in alkaline media and 47 mW/cm2 in acidic media. The detailed investigation on the composition–structure–performance relationship by X‐ray diffraction, X‐ray photoelectron spectroscopy and Mo-ssbauer spectroscopy suggests that Fe‐N4, together with graphitic‐N and pyridinic‐N are the active ORR components. The promising direct methanol fuel cell performance displayed by the Fe‐N‐C catalyst is related to the intrinsic high catalytic activity, and critically for this application, to the high methanol tolerance.
文摘Combustion synthesis involving metallothermic reduction of Fe2O3 and TiO2 was conducted in the mode of self-propagating high-temperature synthesis(SHS)to fabricate FeAl-based composites with dual ceramic phases,TiB2/Al2O3 and TiC/Al2O3.The reactant mixture included thermite reagents of 0.6Fe2O3+0.6TiO2+2Al,and elemental Fe,Al,boron,and carbon powders.The formation of xFeAl−0.6TiB2−Al2O3 composites with x=2.0−3.6 and yFeAl−0.6TiC−Al2O3 composites with y=1.8−2.75 was studied.The increase of FeAl causes a decrease in the reaction exothermicity,thus resulting in the existence of flammability limits of x=3.6 and y=2.75 for the SHS reactions.Based on combustion wave kinetics,the activation energies of Ea=97.1 and 101.1 kJ/mol are deduced for the metallothermic SHS reactions.XRD analyses confirm in situ formation of FeAl/TiB2/Al2O3 and FeAl/TiC/Al2O3 composites.SEM micrographs exhibit that FeAl is formed with a dense polycrystalline structure,and the ceramic phases,TiB2,TiC,and Al2O3,are micro-sized discrete particles.The synthesized FeAl−TiB2−Al2O3 and FeAl−TiC−Al2O3 composites exhibit the hardness ranging from 12.8 to 16.6 GPa and fracture toughness from 7.93 to 9.84 MPa·m1/2.
文摘Iron-based single-atom catalysts with nitrogen-doped carbon as support(Fe-SA/NPC)are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells.However,synthesizing high-loading Fe-SA catalysts by a simple procedure remains challenging.Herein,we report a high-loading(7.5 wt%)Fe-SA/NPC catalyst prepared by carbon-assisted pyrolysis of metal complexes.Both the nitrogen-doped porous carbon(NPC)support with high specific surface area and ο-phenylenediamine(o-PD)play key roles role in the preparation of high-loading Fe-SA/NPC catalysts.The results of X-ray photoelectron spectroscopy,high-angle annular dark-field scanning transmission electron microscopy,and X-ray absorption fine structure spectroscopy experiments show that the Fe atoms are anchored on the carbon carriers in a single-atom site configuration and coordinated with four of the doped nitrogen atoms of the carbon substrates(Fe-N_(4)).The activities of the Fe-SA/NPC catalysts in the oxygen reduction reaction increased with increasing iron loading.The optimized 250Fe-SA/NPC-800 catalyst exhibited an onset potential 0.97 V of and a half-wave potential of 0.85 V.Our study provides a simple approach for the large-scale synthesis of high-loading single-atom catalysts.
文摘The mechanism of idiopathic ventricular tachycardia originating from the right ventricular outflow tract (RVOT) is not clear. Many clinical reports have suggested a mechanism of triggered activity. However, there are few studies investigating this be- cause of the technical difficulties associated with examining this theory. The L-type calcium current (/Ca-L), an important in- ward current of the action potential (AP), plays an important role in arrhythmogenesis. The aim of this study was to explore differences in the APs of right ventricular (RV) and RVOT cardiomyocytes, and differences in electrophysiological character- istics of the ICa-L in these myocytes. Rabbit RVOT and RV myocytes were isolated and their AP and Ic,-L were investigated us- ing the patch-clamp technique. RVOT cardiomyocytes had a wider range of AP duration (APD) than RV cardiomyocytes, with some markedly prolonged APDs and markedly shortened APDs. The markedly shortened APDs in RVOT myocytes were abolished by treatment with 4-AP, an inhibitor of the transient outward potassium current, but the markedly prolonged APDs remained, with some myocytes with a long AP plateau not repolarizing to resting potential. In addition, early afterdepolariza- tion (EAD) and second plateau responses were seen in RVOT myocytes but not in RV myocytes. RVOT myocytes had a high- er current density for/Ca-L than RV myocytes (RVOT (13.16±0.87) pA pF-1, RV (8.59±1.97) pA pF-1; P〈0.05). The ICa-L and the prolonged APD were reduced, and the EAD and second plateau response disappeared, after treatment with nifedipine (10 μmol L^-1), which blocks the Ica-L. In conclusion, there was a wider range of APDs in RVOT myocytes than in RV myocytes, which is one of the basic factors involved in arrhythmogenesis. The higher current density for ICa-L is one of the factors causing prolongation of the APD in RVOT myocytes. The combination of EAD with prolonged APD may be one of the mechanisms of RVOT-VT generation.
基金supported by National Basic Research Program of China (Grant No. 2006CB403200)National Natural Science Foundation of China (Grant No. 41001162)+3 种基金Knowledge Innovation Project of the Chinese Academy of Sciences (Grant No. KZCX2-YW-306)National Key Technology R&D Program (Grant Nos. 2006BAC01A09 and 2008BAD98B07)Provincial Governor Foundation of Guizhou (Grant No. 2010-95)Opening Fund of State Key Laboratory of Environmental Geochemistry (Grant No. SKLEG9008)
文摘Deforestation to reclaim land often triggers severe soil erosion in the Guizhou Karst Plateau. 137Cs dating of the deposited sediments in the karst depression bottom was used to estimate soil losses by surface erosion since deforestation started in 1979 on hillslopes in the Shirenzhai catchment, Puding County, Guizhou Province. The catchment has a drainage area of 0.054 km2. The average 137Cs contents of the top and peak layers in five cores of the depression bottom (with an area of 2652 m2), collected in 2009, were 2.35 and 7.25 Bq kg-1, respectively. The medium depths in the depression (which ranged between 84 cm and 113.5 cm with a mean value of 92.1 cm) showed the presence of sediments deposited in 1979. The total volume and weight of the deposited sediments since 1979 were estimated to be 1965 m3 and 2496 t, respectively. The depression bottom can be treated as a temporary impoundment and its sediment trapping efficiency was estimated to be 0.7. The relevant average soil erosion rate on the hillslopes was 2315 t km-2 yr-1 since 1979. The mean 137Cs inventory of the five cores was 7693 Bq m-2, which was ~10 times the local reference inventory of 782 Bq m-2. The total 137Cs activity of the sediments in the bottom was 20.4×106 Bq, and the relevant 137Cs inventory loss from the hillslopes was 358 Bq m-2 (since 1954), which accounted for 45.8% of the reference inventory. As soil erosion was not severe before and after the period of deforestation and following cultivation in 1979-1990, the erosion rates on the hillslopes could potentially reach 7000 t km-2 yr-1.
基金This work was financially supported by the Ministry of Science and Technology of China (Grants 2012CB215500 and 2013CB933100) and the National Natural Science Foundation of China (Grants 21103178 and 21033009).
文摘A PtFe/C catalyst has been synthesized by impregnation and high-temperature reduction followed by acid-leaching. X-ray diffraction, X-ray photoelectron spectroscopy and X-ray atomic near edge spectroscopy characterization reveal that PtgFe alloy formation occurs during high-temperature reduction and that unstable Fe species are dissolved into acid solution. The difference in Fe concentration from the core region to the surface and strong O-Fe bonding may drive the outward diffusion of Fe to the highly corrugated Pt-skeleton, and the resulting highly dispersed surface FeOx is stable in acidic medium, leading to the construction of a PtBFe@Pt-FeOx architecture. The as prepared PtFe/C catalyst demonstrates a higher activity and comparable durability for the oxygen reduction reaction compared with a Pt/C catalyst, which might be due to the synergetic effect of surface and subsurface Fe species in the PtFe/C catalyst.
基金supported by the National Basic Research Program of China (973 Program, 2015CB351903)the National Key Research and Development Program (2017YFA0207301)+1 种基金the National Natural Science Foundation of China (51402282, 21474095 and 21476104)CAS Key Research Program of Frontier Sciences (QYZDB-SSW-SLH018)
文摘Developing low-cost, high-performance elec- trocatalysts for the oxygen reduction reaction (ORR) is crucial for implementation of fuel cells and metal-air batteries into practical applications. Graphene-based catalysts have been extensively investigated for ORR in alkaline electrolytes. However, their performance in acidic electrolytes still requires further improvement compared to the Pt/C catalyst. Here we report a self-templating approach to prepare graphene-based sandwich-like porous carbon nanosheets for efficient ORR in both alkaline and acidic electrolytes. Graphene oxides were first used to adsorb m-phenylenediamine molecules which can form a nitrogen-rich polymer network after oxidative poly- merization. Then iron (Fe) salt was introduced into the polymer network and transformed into ORR active Fe-N-C sites along with Fe, FeS, and FEN0.05 nanopartides after pyr- olysis, generating ORR active sandwich-like carbon na- nosheets. Due to the presence of multiple ORR active sites. The as-obtained catalyst exhibited prominent ORR activity with a half-wave potential -30 mV more positive than Pt/C in 0.1 mol L-1 KOH, while the half-wave potential of the catalyst was only -40 mV lower than that of commercial Pt/C in 0.1 mol L-1 HClO4. The unique planar sandwich-like structure could expose abundant active sites for ORR. Meanwhile, the graphene layer and porous structure could simultaneously enhance electrical conductivity and facilitate mass transport. The prominent electrocatalytic activity and durability in both alkaline and acidic electrolytes indicate that these carbon na- nosheets hold great potential as alternatives to precious metal- based catalysts, as demonstrated in zinc-air batteries and proton exchange membrane fuel cells.
文摘In energy industries, it is always of difficulty to produce high heat value(HHV) gas continuously using pulverized coal. In this paper, a new type furnace for partitioned alternative gasification using pulverized coal is developed, in which the oxidation and reduction reaction occur alternatively with the dropping of pulverized coal and finally HHV gas could be continuously obtained at the reduction zone exit and low heat value(LHV) gas at the oxidation zone exit. Furthermore, the gasification characteristics and their factors in furnace are numerically simulated under two dimensional model with a self-coded program, based on heat, mass and energy transfer as well as reaction principles. It is found that the producing rate of HHV gas is 1.10Nm3/kg with heat value of ll.72MJ/Nm3, how- ever, that of LHV gas is 2.58Nm3/kg with heat value of 5.30MJ/Nm3, and the coal gas efficiency is 81.16% under optimized conditions.
基金jointly supported by the National Key Research and Development Program of China(2017YFA0206500and 2018YFA0209103)the National Natural Science Foundation of China(21832003,21773111,51571110 and 21573107)the Fundamental Research Funds for the Central Universities(020514380126)
文摘Cobalt-based oxygenic compounds Co(OH)2,CoO and Co3 O4 are attractive for electrochemical energy storage owing to their high theoretical capacities and pseudocapacitive properties.Despite the great efforts to their compositional and morphological regulations,the performances to date are still quite limited owing to the low active surface area and sluggish charge transfer kinetics.Herein,different Co-based nanocrystals(Co-NCs)were conveniently anchored on the hierarchical nitrogen-doped carbon nanocages(hNCNCs)with high specific surface area and coexisting micro-meso-macropores to decrease the size and facilitate the charge transfer.Accordingly,a high specific capacity of1170 Fg^-1 is achieved at 2 Ag^-1 for the Co(OH)2/hNCNCs hybrid,in which the capacitance of Co(OH)2(2214 F gco(OH)2)is approaching to its theoretical maximum(2595 Fg^-1),demonstrating the high utilization of active materials by the hybridization with N-doped nanocarbons.This study also reveals that these Co-NCs store/release electrical energy via the same reversible redox reaction despite their different pristine compositions.This insight on the energy storage of Co-based nanomaterials suggests that the commonly-employed transformation of the Co-NCs from Co(OH)2 to CoO and Co3 O4 on carbon supports is unnecessary and even could be harmful to the energy storage performance.The result is instructive to develop high-energy-density electrodes from transition metal compounds.
基金supported by the National Natural Science Foundation of China(51272155,21875061,21975066 and 21901157)the Open Research Fund Program of Science and Technology on Aerospace Chemical Power Laboratory(STACPL 120201B05)the National Key R&D Program of China(2021YFC2100100)。
文摘The rechargeable aluminum-sulfur(Al-S)battery is a promising alternative-energy storage device with high energy density and made of cheap raw materials.However,Al-S batteries face several obstacles,especially the shuttle effect.Herein,a binder-free S@Ti_(3)C_(2)T_(x)sandwich structure film with uniform sulfur dispersion was designed.The two-dimensional(2D)layered material Ti_(3)C_(2)T_(x) not only has the function of binder and conductive agent but also is a promising host for sulfur anchoring.As a result,S@Ti_(3)C_(2)T_(x)film showed an initial capacity of 489 mA h g^(−1)at 300 mA g^(−1) and retained the value at 415 mA h g^(−1)after 280 stable cycles,with an average Coulombic efficiency of~95%.The film displayed higher capacity and stability than the S+Ti_(3)C_(2)T_(x)cathode prepared by the slurry-coating method(the initial capacity was 317 mA h g^(−1)and then decayed to 222 mA h g^(−1) after 160 cycles).The main capacity of S@Ti_(3)C_(2)T_(x) film in the Al-S battery came from the reversible redox reaction of S^(2−) and S.This new 2D material combined with a controllable electrode structure design paves the way for the development of Al-S batteries.
文摘Hierarchical TiO2 photocatalysts with a one-dimensional heterojunction were synthesized via a facile template-free hydrothermal method. The TiO2 photo- catalysts were flower-like microspheres with a 3 μm diameter. The base structure of the flower-like microspheres was a uniform nanowire with a 10 nm diameter. Anatase films were evenly coated onto the surface of the rutile TiO2 nanowires to form a one-dimensional core--shell base structure. This kind of one-dimensional heterojunction is conducive to the separation of charge carriers. In addition, the hierarchical TiO2 microspheres possessed a good mesoporous structure with a high specific surface area of 260 m2/g. Thus, the light scattering and utilization efficiency were improved in this structure. The photocatalysts exhibited better performance in both photocatalytic oxidation and reduction reactions. Moreover, the novel TiO2 photocatalysts displayed excellent stability in these reactions. This kind of hierarchical TiO2 structure has never been reported in the literature. The hierarchical structure and one-dimensional heterojunction were vital to the increase in quantum efficiency. Therefore, these hierarchical TiO2 photocatalysts have potential applications in the environmental and energy fields, such as in photocatalytic degradation, hydrogen production, Li-ion batteries, and dye-sensitized solar cells.
基金supported by the National Natural Science Foundation of China (21525626 and 21761132023)the Program of Introducing Talents of Discipline to Universities (BP0618007)。
文摘Designing highly selective and efficient singleatom electrocatalysts is essential for ammonia production under ambient conditions. This paper describes a density functional theory study on exploring the performance trends of transition metal complexes with P-based ligands in nitrogen reduction reaction(NRR) and further develops a design principle for high-performance single-atom catalysts(SACs)of NRR. Among the explored catalysts, W@BP(0.40 eV),Ta@BP(0.47 eV), and Nb@BP(0.53 eV) are identified as remarkable candidates with low free energy change in the potential-limiting step, high stability and high electrical conductivity for NRR. It is worth noting that almost all SACs with P-based ligands exhibit high NRR selectivity, due to the fact that they adsorb *N_(2) more strongly than *H. The adsorption free energy of *N_(2) H can be considered as a descriptor for the intrinsic activity trends in NRR. Furthermore, by constructing a volcano plot of the activity against the electronic charge on metal centers, it is demonstrated that the metal center with a moderate amount of positive charge can promote the catalytic performance of NRR.