Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electro...Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electrocatalytic oxidations of saturated alcohols(C_(1)-C_(6))to selectively form formate using Ni Co hydroxide(Ni Co-OH)derived Ni Co_(2)O_(4)solid-acid electrocatalysts with balanced Lewis acid(LASs)and Brønsted acid sites(BASs).Thermal treatment transforms BASs-rich(89.6%)Ni Co-OH into Ni Co_(2)O_(4)with nearly equal distribution of LASs(53.1%)and BASs(46.9%)which synergistically promote adsorption and activation of OH-and alcohol molecules for enhanced oxidation activity.In contrast,BASs-enriched Ni Co-OH facilitates formation of higher valence metal sites,beneficial for water oxidation.The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6alcohols increases as increased number of hydroxyl groups and decreased HOMO-LUMO gaps:methanol(C_(1))<ethylene glycol(C_(2))<glycerol(C3)<meso-erythritol(C4)<xylitol(C5)<sorbitol(C6),while the formate selectivity shows the opposite trend from 100 to 80%.This study unveils synergistic roles of LASs and BASs,as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.展开更多
Peroxymonosulfate(PMS)-based advanced oxidation technology has been proven to be a viable option for the decontamination of organic pollutants from water bodies.Advanced catalyst design is essential to this technology...Peroxymonosulfate(PMS)-based advanced oxidation technology has been proven to be a viable option for the decontamination of organic pollutants from water bodies.Advanced catalyst design is essential to this technology.Herein,a vanadium-doped LaFeO_(3) perovskite(LFO-V)featuring asymmetric Fe-O-V sites was rationally designed.Thanks to orbital electron interaction between Fe and V atoms,the modified electronic structure elevated electron density near the Fermi energy level while reducing the energy barrier toward effective PMS activation.This facilitated concurrent PMS reduction at the Fe sites to generate SO_(4)^(·-)and·OH(57.7%),and PMS oxidation at V sites to produce ^(1)O_(2)(42.3%).The LFO-V/PMS system demonstrated excellent tetracycline(TC)degradation performance with a 2-fold enhancement in rate constant compared to that of pristine LFO.Further,the LFO-V maintained long-term stability,and the toxicity of degradation intermediates was evaluated through microbial metabolomics.This work establishes an effective route to regulate the PMS activation pathways through precise electronic structure modulation,advancing the rational design of advanced Fenton-like catalysts.展开更多
Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization w...Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar(MHC)for Fenton-like degradation of tetracycline in aqueous solution.Diverse shapes of Fe_(3)O_(4) and nano zero-valent iron(nZVI)were doped with abundant oxygen containing groups and persistent free radicals(PFRs).Multiple catalysis sites including iron species,PFRs,oxygen containing groups,and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect.Notably,MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L,with a total organic carbon(TOC)removal rate of 35%.Furthermore,after four cycles of reuse,the degradation efficiency slightly decreased to 93%.This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.展开更多
Large-scale CO_(2)emissions have exacerbated the greenhouse effect,reinforcing the critical need for efficient CO_(2)mitigation methods.Plasma-catalytic technology enables CO_(2)conversion under mild conditions,especi...Large-scale CO_(2)emissions have exacerbated the greenhouse effect,reinforcing the critical need for efficient CO_(2)mitigation methods.Plasma-catalytic technology enables CO_(2)conversion under mild conditions,especially for CO_(2)methanation(the Sabatier reaction),which has attracted significant attention due to its economic benefits and the potential for safe energy transportation via existing natural gas pipelines.The development of high-performance CO_(2)methanation catalysts remains an ongoing and long-term objective,and there is a lack of adequate in-situ characterization techniques to investigate the mechanisms.This study focuses on the Ni/La_(2)O_(3)(LN)catalyst and introduces two CO_(2)activation strategies through F and Na modifications:the Ni-Ov-Ni site activation with electron transfer from Ni0 under low-power conditions and basic site activation under high-power conditions.The LN-NaF catalysts enhance CO_(2)methanation activity across the entire power range compared to LN,achieving a CO_(2)conversion of 86.3%and CH4 selectivity of 99.4%.Additionally,LN-F(h)reaches a CH4 yield 4.15 times higher than that of LN at low power.Furthermore,in-situ diffuse reflectance infrared Fourier transform(DRIFT)spectroscopy with a self-made reactor are performed under plasma-catalytic conditions to reveal the CO_(2)adsorption and conversion mechanisms,indicating that different dopants(F,Na,and NaF)exhibit promoting effects on different intermediates,resulting in variations in CO_(2)methanation activity.This study provides valuable insights for improving catalyst performance and a thorough comprehension of mechanisms in CO_(2)methanation.展开更多
Molecular recognition of bioreceptors and enzymes relies on orthogonal interactions with small molecules within their cavity. To date, Chinese scientists have developed three types of strategies for introducing active...Molecular recognition of bioreceptors and enzymes relies on orthogonal interactions with small molecules within their cavity. To date, Chinese scientists have developed three types of strategies for introducing active sites inside the cavity of macrocyclic arenes to better mimic molecular recognition of bioreceptors and enzymes.The editorial aims to enlighten scientists in this field when they develop novel macrocycles for molecular recognition, supramolecular assembly, and applications.展开更多
Single atom catalysts supported by two-dimensional(2D)materials,including graphene,g-C_(3)N_(4),and graphdiyne,ex-hibit promising electrocatalytic nitrogen reduction reaction(NRR)activity.Nevertheless,sometimes theore...Single atom catalysts supported by two-dimensional(2D)materials,including graphene,g-C_(3)N_(4),and graphdiyne,ex-hibit promising electrocatalytic nitrogen reduction reaction(NRR)activity.Nevertheless,sometimes theoretical works failed to predict the high activity of NRR of single atom cat-alysts,especially for Fe,Co,Mn,Cu,Ru.In this work,based on DFT calculations,it is suggested that dual-atom sites on N doped graphene(M_(2)@N-graphene)rather than single-atom sites are more likely to be the active sites for NRR.Notably,Fe_(2)@N_(3),Co_(2)@N_(2),Mn_(2)@N_(2),Cu_(2)@N_(1),and Ru_(2)@N_(3)endow the best catalytic activity with corresponding limiting potentials of-0.26,-0.18,-0.17,-0.39,and-0.30 V,re-spectively.Furthermore,on g-C_(3)N_(4)and graphdiyne,triple-atom sites(TAS,M_(3))such as Ru_(3)(Co_(3))@g-C_(3)N_(4)and Ru_(3)(Rh_(3))@graphdiyne are expected to exhibit higher stability and NRR catalytic performance than single-atom sites(SAS)and dual-atom sites(DAS),with corresponding limiting potentials of-0.28,-0.48,-0.24,and-0.23 V.The calculated results with the corresponding experimental potentials indicate that the origin of superior NRR ac-tivity observed in experiments may be contributed by M_(2)or M_(3)on 2D materials.This study provides an in-depth investigation into real active NRR sites of metal atoms supported on 2D materials and contributes to the design of effective NRR catalysts.展开更多
Gallium nitride(GaN)single crystal with prominent electron mobility and heat resistance have great potential in the high temperature integrate electric power systems.However,the sluggish charge storage kinetics and in...Gallium nitride(GaN)single crystal with prominent electron mobility and heat resistance have great potential in the high temperature integrate electric power systems.However,the sluggish charge storage kinetics and inadequate energy densities are bottlenecks to its practical application.Herein,the self-supported GaN/Mn_(3)O_(4) integrated electrode is developed for both energy harvesting and storage under the high temperature environment.The experimental and theoretical calculations results reveal that such integrated structures with Mn-N heterointerface bring abundant active sites and reconstruct low-energy barrier channels for efficient charge transferring,reasonably optimizing the ions adsorption ability and strengthening the structural stability.Consequently,the assembled GaN based supercapacitors deliver the power density of 34.0 mW cm^(-2) with capacitance retention of 81.3%after 10000 cycles at 130℃.This work innovatively correlates the centimeter scale GaN single crystal with ideal theoretical capacity Mn_(3)O_(4) and provides an effective avenue for the follow-up energy storage applications of the wide bandgap semiconductor.展开更多
Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high curr...Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high current densities.Herein,a Pr-doped Co(OH)_(2)hexagonal sheet(Pr/Co=1/9,in mole)is synthesized by electrodeposition as highly performant catalyst for 5-hydroxymethylfurfural(HMF)oxidation reaction(HMFOR)to produce 2,5-furandicarboxylic acid(FDCA).This novel and low-cost catalyst possesses a rather low onset potential of 1.05 V(vs.RHE)and requires only 1.10 V(vs.RHE)to reach a current density of 10 mA cm^(-2)for HMFOR,significantly outperforming Co(OH)_(2)benchmark(i.e.,210 mV higher to reach10 m A cm^(-2)).The origin of Pr promotion effect as well as the evolution of CoOOH catalytic sites and HMFOR process has been deeply elucidated by physical characterizations,kinetic experiments,in situ electrochemical techniques,and theoretical calculations.The unique Pr-ameliorated CoOOH active centers enable 100%conversion of HMF,99.6%selectivity of FDCA,and 99.7%Faraday efficiency,with a superior cycling durability toward HMFOR.This can be one of the most outstanding results for Co-based HMFOR catalysts to date in the literature.Thereby this work can help open up new horizons for constructing novel and efficient Co-based electrocatalysts by the utilization of lanthanide elements.展开更多
Herein,a new type of two-dimensional(2D)/2D Ti_(3)C_(2)/TiO_(2) heterojunction was developed for efficient photocatalytic nitrogen reduction reaction(NRR),in which TiO_(2) nanosheets(TiO_(2) Ns)were designed as the ma...Herein,a new type of two-dimensional(2D)/2D Ti_(3)C_(2)/TiO_(2) heterojunction was developed for efficient photocatalytic nitrogen reduction reaction(NRR),in which TiO_(2) nanosheets(TiO_(2) Ns)were designed as the main catalyst,while Ti_(3)C_(2) MXene served as the co-catalyst.Experimental and theoretical results revealed that Ti_(3)C_(2) MXene introduced electron-rich unsaturated Ti sites,serving as highly active sites for both the adsorption and activation of N_(2) on the Ti_(3)C_(2)/TiO_(2) heterojunction.Furthermore,the 2D/2D Ti_(3)C_(2)/TiO_(2) heterostructure greatly promoted the directional separation and transfer of charge carriers,facilitated by the internal electric field.This structural feature enabled the spatial separation of the N_(2) reduction and H2 O oxidation half-reactions on the distinct surfaces of Ti_(3)C_(2)(001)and TiO_(2)(001),con-sequently reducing the reaction energy barrier for each respective process.The synergistic effects arising from the interface and surface interactions within the heterojunction conspicuously improved the photo-catalytic NRR activity.As a result,the optimized Ti_(3)C_(2)/TiO_(2) heterojunction exhibited a high NH_(3) produc-tion rate of 24.4μmol g−1 h−1 in the absence of sacrificial agents,representing a remarkable 12.8-fold increase compared to individual TiO_(2) Ns.This work provides new insights into rational design of high-performance heterogeneous photocatalysts and offers a deeper understanding of the mechanism under-lying surface active sites in the photocatalytic NRR process.展开更多
Cu/ZnO-based catalysts are widely employed for methanol synthesis via CO_(2) hydrogenation.The preparation procedure is sensitive to the particle size and interfacial structure,which are considered as potential active...Cu/ZnO-based catalysts are widely employed for methanol synthesis via CO_(2) hydrogenation.The preparation procedure is sensitive to the particle size and interfacial structure,which are considered as potential active centers influencing the rate of both methanol and CO formation.The particle size and the interaction between Cu and the support materials are influenced by the coprecipitation conditions,let alone that the mechanistic divergence remains unclear.In this work,a series of Cu/ZnO/ZrO_(2) catalysts were prepared via co-precipitation at different pH value and systematically characterized.The structure has been correlated with kinetic results to establish the structure-performance relationship.Kinetic analysis demonstrates that methanol synthesis follows a single-site Langmuir-Hinshelwood(L-H)mechanism,i.e.,Cu serves as the active site where CO_(2) and H_(2) competitively adsorb and react to form methanol.In contrast,CO formation proceeds via a dual-site L-H mechanism,where CO_(2) adsorbs onto ZnO and H_(2) onto Cu,with the reaction occurring at the Cu/ZnO interface.Therefore,for the direct formation of methanol,solely reducing the particle size of Cu would not be beneficial.展开更多
The kidney is essential for maintaining fluid,electrolyte,and metabolite homeostasis,and for regulating blood pressure.The pig serves as a valuable biomedical model for human renal physiology,offering insights across ...The kidney is essential for maintaining fluid,electrolyte,and metabolite homeostasis,and for regulating blood pressure.The pig serves as a valuable biomedical model for human renal physiology,offering insights across different physiological states.In this study,single-cell RNA sequencing was used to profile 138469 cells from 12 pig kidney samples collected during the embryonic(E),fattening(F),and pregnancy(P)periods,identifying 29 cell types.Proximal tubule(PT)cells exhibited elevated expression of metabolism-related transcription factors(TFs),including GPD1,ACAA1,and AGMAT,with validation across multiple individuals,periods,and species.Fluorescence homologous double-labeling of paraffin sections further confirmed the expression of ACAA1 and AGMAT in PT cells.Comparative analysis of pig and human kidneys revealed a high degree of similarity among corresponding cell types.Analysis of cell-type heterogeneity highlighted the diversity of thick ascending limb(TAL)cells,identifying a TAL subpopulation related to immune function.Additionally,the functional heterogeneity of kidney-resident macrophages(KRM)was explored across different anatomical sites.In the renal medulla,KRM were implicated in phagocytosis and leukocyte activation,whereas in the renal pelvis,they functioned as ligands,recruiting neutrophils with bactericidal activity to the renal pelvis to combat urinary tract infections.展开更多
The type and quantity of active sites on a catalyst surface determine catalytic activity.In this study,machine learning was employed to assist in the construction of C=O and pyridine N active sites using sludge waste....The type and quantity of active sites on a catalyst surface determine catalytic activity.In this study,machine learning was employed to assist in the construction of C=O and pyridine N active sites using sludge waste.Reactive descriptors,including C%,N%,O%,Fe%,pyrolysis temperature,heating rate,and pyrolysis time were proposed.Decision tree,extra tree,extreme gradient boosting(XGB),automatic relevance determination,and Bayesian ridge regression models were constructed and optimized.Among these,the XGB model was demonstrated with superior accuracy for prediction of C=O sites on the catalyst surface.Additionally,an ensemble model combining extra trees and XGB was developed to predict pyridine N,with R~2 value as high as 0.80 and minimum root mean square error(RMSE)of 0.1386.The ensemble model demonstrated a 17%improvement in accuracy compared to individual models.The model enables high-throughput screening of construction conditions for C=O and pyridine N.The study found that a pyrolysis temperature above of 500–800℃,a heating rate of 10–20℃/min,and a heating time of 120–200 min favor the generation of C=O active sites.For pyridine N sites,a pyrolysis temperature between 400℃ and 600℃,a heating rate of 5–10℃/min,and a pyrolysis time of around 150 min are optimal.Experimental validation demonstrated that both models exhibit excellent predictive performance,with prediction errors below 10%in all cases.This research provides a method to assist in the construction of C=O and pyridine N active sites,which is beneficial for guiding the design of sludge catalysts.展开更多
In Lima(the capital of Peru),archaeological sites are constantly being threatened by accelerated urban expansion.This study examines Independencia(a district in northern Lima),where 95%of archaeological areas have bee...In Lima(the capital of Peru),archaeological sites are constantly being threatened by accelerated urban expansion.This study examines Independencia(a district in northern Lima),where 95%of archaeological areas have been encroached upon due to inadequate planning and conservation policies.Focusing on four key archaeological sites(Cerro La Cruz,Cerro San Jerónimo,Pampa de Cueva,and San Jerónimo),this study employed a comprehensive pathological analysis to assess the extent and causes of deterioration.Data were gathered through field observation sheets based on the Ministry of Culture’s Conservation Guide,alongside historical photographs,aerial imagery,and urban mapping.The results indicate that human agents(27.1%)are the primary drivers of damage,supplemented by fortuitous(4.07%)and biological(2.89%)agents.The pronounced deterioration,particularly from human agents,underscores the urgent need for a holistic conservation strategy that integrates community participation with technical heritage management,ensuring that Lima’s pre-Hispanic legacy is preserved amidst ongoing urban pressure.展开更多
Two protected sites located on the outskirts of the Sena Oura National Park (PNSO) in West Mayo-Kebbi cover an area of 1800 m2 is pattern choose in pastoral enclave in both village. This study was undertaken to highli...Two protected sites located on the outskirts of the Sena Oura National Park (PNSO) in West Mayo-Kebbi cover an area of 1800 m2 is pattern choose in pastoral enclave in both village. This study was undertaken to highlight the floristic diversity of the herbaceous and woody vegetation on these sites in the offing to know the ability of charge into UBT that most support the park peripheral. It took place on two experimental sites on a natural course in two villages: Wazetelan and Massang. The approach used for the study was a survey using the systematic sampling method and a 30 m × 30 m plot. The survey consisted in listing all the taxa in a floristically homogeneous plot, each assigned the Braun-Blanquet dominance abundance coefficient. These surveys revealed a floristic richness of 73 species, 58 genera, including 46 herbaceous and 26 woody species. The Shannon result gives H1' = 0.12 bit for herbaceous species and H2' = 0.44 bit for woody species, meaning that the herbaceous and woody populations of all the surveys have a very low species diversity, as H' < 3 according to the Shannon index assessment threshold. Herbaceous species are divided into 13 families and 33 genera. The most represented families are Fabaceae (27.3%) and Poaceae (21.9%). Most of the other families (1.3%) have only one species, if any. Herbaceous species are divided into 33 genera grouped into 13 families. The most represented families are Fabaces (16 species), 34%, and Poaceae (12 species), 26%. The 26 woody species, most of which come from itinerant surveys, are distributed across 24 genera and 12 families, the most important of which is Fabaceae with 09 species (34.6%). This floristic assessment, in terms of quantity and quality, has enabled us to estimate the carrying capacity of the two pastoral enclaves in Dari and Goumadji cantons, and to guide the government’s actions with regard to rangeland management.展开更多
As an important pillar of China's industrialization process,the coal industry has not only made contributions to economic growth,but also left a large number of coal mine sites bearing historical memories.These si...As an important pillar of China's industrialization process,the coal industry has not only made contributions to economic growth,but also left a large number of coal mine sites bearing historical memories.These sites are not only the witness of the industrial civilization,but also the potential resources for urban renewal and industrial transformation.展开更多
Disrupting the symmetric electron distribution of porphyrin-like Fe singleatom catalysts has been considered as an effective way to harvest high intrinsic activity.Understanding the catalytic performance governed by g...Disrupting the symmetric electron distribution of porphyrin-like Fe singleatom catalysts has been considered as an effective way to harvest high intrinsic activity.Understanding the catalytic performance governed by geometric microstrains is highly desirable for further optimization of such efficient sites.Here,we decipher the crucial role of local microstrain in boosting intrinsic activity and durability of asymmetric Fe single-atom catalysts(Fe-N_(3)S_(1))by replacing one N atom with S atom.The high-curvature hollow carbon nanosphere substrate introduces 1.3%local compressive strain to Fe-N bonds and 1.5%tensile strain to Fe-S bonds,downshifting the d-band center and accelerating the kinetics of*OH reduction.Consequently,highly curved Fe-N_(3)S_(1)sites anchored on hollow carbon nanosphere(FeNS-HNS-20)exhibit negligible current loss,a high half-wave potential of 0.922 V vs.RHE and turnover frequency of 6.2 e^(−1)s^(−1)site−1,which are 53 mV more positive and 1.7 times that of flat Fe-N-S counterpart,respectively.More importantly,multiple operando spectroscopies monitored the dynamic optimization of strained Fe-N_(3)S_(1)sites into Fe-N_(3)sites,further mitigating the overadsorption of*OH intermediates.This work not only sheds new light on local microstrain-induced catalytic enhancement,but also provides a plausible direction for optimizing efficient asymmetric sites via geometric configurations.展开更多
Enhancing the catalytic hydrolysis efficiency of microcystins(MCs)at ambient temperature has been a persistent challenge in water treatment.We employed N_(2)/low-temperature plasma technology to modify the surface of ...Enhancing the catalytic hydrolysis efficiency of microcystins(MCs)at ambient temperature has been a persistent challenge in water treatment.We employed N_(2)/low-temperature plasma technology to modify the surface of natural pyrites(NP),and the resulting nitrogenmodified pyrites(NPN)with a nanorod structure and new Fe-Nx sites are more efficient for the hydrolysis of microcystins-LR(MC-LR).Kinetic experiments revealed that NPN exhibited significantly higher hydrolysis activity(k_(obs)=0.1471 h^(-1))than NP(0.0914 h^(-1)).Liquid chromatography-mass spectrometry(LC/MS)for the intermediates produced by hydrolyzing MC-LR,in situ attenuated total reflectance Fourier transform infrared spectroscopy(in situ ATR-FTIR)and X-ray photoelectron spectroscopy(XPS)analysis unfolded that the Fe and N atoms of Fe-Nx sites on the surface act of NPN as Lewis acid and Bronsted basic respectively,selectively breaking amide bond on MC-LR molecule.This study demonstrates the effectiveness of plasma technology in modifying mineral materials to enhance their catalytic activity,providing a new method for eliminating MCs in practical water treatment.展开更多
Atomic hydrogen(H∗)plays a crucial role in electrochemical reduction technology towards various environmental and energy applications,but suffers from low utilization efficiency arisen from the undesirable H-H dimeriz...Atomic hydrogen(H∗)plays a crucial role in electrochemical reduction technology towards various environmental and energy applications,but suffers from low utilization efficiency arisen from the undesirable H-H dimerization and the competitive adsorption between water molecule with reactants on the traditional adjacent catalytic sites.Herein,we anchored Pd single atoms on the naturally formed titanium oxide of titanium foam to construct Pd_(1)-O-Ti dual-site electrocatalyst with spatially isolated water dissociation and H∗utilization site,which synchronously inhibits the H-H dimerization and the competitive adsorption of water molecule and targeted reactants.Experiments and theoretical calculations revealed that the Ti-O sites could synergistically dissociate water to H∗,which overflowed to nearby Pd single-atom sites for designed reduction reactions and utilization benefiting from the hydrogen spillover ability of titanium oxide substrate.These Pd_(1)-O-Ti dual sites delivered almost 100%bromate reduction efficiency with a rate constant of 1.57 h^(-1),far superior to those of Pdn-O-Ti with adjacent Pd sites(0.52 h^(-1)),Pd_(1)-N-C with single sites(0.04 h^(-1))and commercial Pd/C(0.18 h^(-1)),respectively.This study sheds light on the importance of integrating synergistic active sites for complicated electrochemical reactions,and provide new insights in improving H∗ utilization for environmental remediation.展开更多
Ground response analysis and determination of site-specific ground motion parameters are necessary for evaluating seismic loads to enable sustainable design of aboveground and underground structures,particularly in de...Ground response analysis and determination of site-specific ground motion parameters are necessary for evaluating seismic loads to enable sustainable design of aboveground and underground structures,particularly in deep overburden sites.This study investigates the influence of bedrock interface conditions and depth of soil deposits on obtained site-specific ground motion parameters.Employing the one-dimensional seismic response analysis program SOILQUAKE,the ground responses of five representative soil profiles and 1050 case studies are calculated considering three different site models of seismic input interfaces.The analysis employs the actual bedrock interface with a shear wave velocity of 760 m/s as the reference input bedrock interface.The results illustrate that the selection of the bedrock interface condition significantly affects the seismic response on the ground surface of deep overburden sites.Specifically,the ground surface acceleration response spectra at longer periods are notably smaller compared to those at the actual bedrock site.This may present a challenge for designing long-period high-rise buildings situated in deep overburden sites.It is recommended to select a seismic input bedrock interface closely approximating the actual bedrock depth when conducting seismic response analyses for deep overburden sites.展开更多
Photocatalytic CO_(2)reduction reaction(CO_(2)RR)is one of the promising strategies for sustainably producing solar fuels.The precise identification of catalytic sites and the enhancement of photocatalytic CO_(2)conve...Photocatalytic CO_(2)reduction reaction(CO_(2)RR)is one of the promising strategies for sustainably producing solar fuels.The precise identification of catalytic sites and the enhancement of photocatalytic CO_(2)conversion is imperative yet quite challenging.This critical review summarizes recent advances in porous photo-responsive polymers,including covalent organic frameworks(COFs),covalent triazine frameworks(CTFs),and conjugated microporous polymers(CMPs),those can be rationally designed from the molecular level for visible-light-driven photocatalytic CO_(2)reduction.Additionally,special emphasis is placed on how the well-defined active sites on these polymers can influence their properties and photocatalytic performance.The precise regulation and control of microenvironments and electronic properties of metal active centers are crucial for boosting catalytic efficiency and selectivity,as well as for the design of better photocatalysts for CO_(2)reduction.展开更多
基金the financial support from the National Natural Science Foundation of China(52172110,52472231,52311530113)Shanghai"Science and Technology Innovation Action Plan"intergovernmental international science and technology cooperation project(23520710600)+1 种基金Science and Technology Commission of Shanghai Municipality(22DZ1205600)the Central Guidance on Science and Technology Development Fund of Zhejiang Province(2024ZY01011)。
文摘Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electrocatalytic oxidations of saturated alcohols(C_(1)-C_(6))to selectively form formate using Ni Co hydroxide(Ni Co-OH)derived Ni Co_(2)O_(4)solid-acid electrocatalysts with balanced Lewis acid(LASs)and Brønsted acid sites(BASs).Thermal treatment transforms BASs-rich(89.6%)Ni Co-OH into Ni Co_(2)O_(4)with nearly equal distribution of LASs(53.1%)and BASs(46.9%)which synergistically promote adsorption and activation of OH-and alcohol molecules for enhanced oxidation activity.In contrast,BASs-enriched Ni Co-OH facilitates formation of higher valence metal sites,beneficial for water oxidation.The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6alcohols increases as increased number of hydroxyl groups and decreased HOMO-LUMO gaps:methanol(C_(1))<ethylene glycol(C_(2))<glycerol(C3)<meso-erythritol(C4)<xylitol(C5)<sorbitol(C6),while the formate selectivity shows the opposite trend from 100 to 80%.This study unveils synergistic roles of LASs and BASs,as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.
基金supported by the National Natural Science Foundation of China(Nos.W2412093 and 52170068)the Fundamental Research Funds for the Central Universities(No.DUT24RC(3)079).
文摘Peroxymonosulfate(PMS)-based advanced oxidation technology has been proven to be a viable option for the decontamination of organic pollutants from water bodies.Advanced catalyst design is essential to this technology.Herein,a vanadium-doped LaFeO_(3) perovskite(LFO-V)featuring asymmetric Fe-O-V sites was rationally designed.Thanks to orbital electron interaction between Fe and V atoms,the modified electronic structure elevated electron density near the Fermi energy level while reducing the energy barrier toward effective PMS activation.This facilitated concurrent PMS reduction at the Fe sites to generate SO_(4)^(·-)and·OH(57.7%),and PMS oxidation at V sites to produce ^(1)O_(2)(42.3%).The LFO-V/PMS system demonstrated excellent tetracycline(TC)degradation performance with a 2-fold enhancement in rate constant compared to that of pristine LFO.Further,the LFO-V maintained long-term stability,and the toxicity of degradation intermediates was evaluated through microbial metabolomics.This work establishes an effective route to regulate the PMS activation pathways through precise electronic structure modulation,advancing the rational design of advanced Fenton-like catalysts.
基金supported byHainan Provincial Natural Science Foundation of China(Nos.422RC600,519QN175)National Natural Science Foundation ofChina(Nos.52160018,21801053,52400206,52500209)High-Level Talent Program of Hainan Province(Nos.XJ2400008202,XJ2400011473).
文摘Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar.In this paper,a K_(2)FeO_(4)-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar(MHC)for Fenton-like degradation of tetracycline in aqueous solution.Diverse shapes of Fe_(3)O_(4) and nano zero-valent iron(nZVI)were doped with abundant oxygen containing groups and persistent free radicals(PFRs).Multiple catalysis sites including iron species,PFRs,oxygen containing groups,and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect.Notably,MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L,with a total organic carbon(TOC)removal rate of 35%.Furthermore,after four cycles of reuse,the degradation efficiency slightly decreased to 93%.This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.
基金supported by the National Natural Science Foundation of China(No.51878292).
文摘Large-scale CO_(2)emissions have exacerbated the greenhouse effect,reinforcing the critical need for efficient CO_(2)mitigation methods.Plasma-catalytic technology enables CO_(2)conversion under mild conditions,especially for CO_(2)methanation(the Sabatier reaction),which has attracted significant attention due to its economic benefits and the potential for safe energy transportation via existing natural gas pipelines.The development of high-performance CO_(2)methanation catalysts remains an ongoing and long-term objective,and there is a lack of adequate in-situ characterization techniques to investigate the mechanisms.This study focuses on the Ni/La_(2)O_(3)(LN)catalyst and introduces two CO_(2)activation strategies through F and Na modifications:the Ni-Ov-Ni site activation with electron transfer from Ni0 under low-power conditions and basic site activation under high-power conditions.The LN-NaF catalysts enhance CO_(2)methanation activity across the entire power range compared to LN,achieving a CO_(2)conversion of 86.3%and CH4 selectivity of 99.4%.Additionally,LN-F(h)reaches a CH4 yield 4.15 times higher than that of LN at low power.Furthermore,in-situ diffuse reflectance infrared Fourier transform(DRIFT)spectroscopy with a self-made reactor are performed under plasma-catalytic conditions to reveal the CO_(2)adsorption and conversion mechanisms,indicating that different dopants(F,Na,and NaF)exhibit promoting effects on different intermediates,resulting in variations in CO_(2)methanation activity.This study provides valuable insights for improving catalyst performance and a thorough comprehension of mechanisms in CO_(2)methanation.
文摘Molecular recognition of bioreceptors and enzymes relies on orthogonal interactions with small molecules within their cavity. To date, Chinese scientists have developed three types of strategies for introducing active sites inside the cavity of macrocyclic arenes to better mimic molecular recognition of bioreceptors and enzymes.The editorial aims to enlighten scientists in this field when they develop novel macrocycles for molecular recognition, supramolecular assembly, and applications.
基金partially supported by the National Natural Science Foundation of China(Nos.22373092,22288201)CAS Project for Young Scientists in Basic Research(YSBR-051)+1 种基金Innovation Program for Quantum Science and Technology(2021ZD0303306)supported by University of Science and Technology of China Tang Scholarship and State Scholarship Fund(202206345005)。
文摘Single atom catalysts supported by two-dimensional(2D)materials,including graphene,g-C_(3)N_(4),and graphdiyne,ex-hibit promising electrocatalytic nitrogen reduction reaction(NRR)activity.Nevertheless,sometimes theoretical works failed to predict the high activity of NRR of single atom cat-alysts,especially for Fe,Co,Mn,Cu,Ru.In this work,based on DFT calculations,it is suggested that dual-atom sites on N doped graphene(M_(2)@N-graphene)rather than single-atom sites are more likely to be the active sites for NRR.Notably,Fe_(2)@N_(3),Co_(2)@N_(2),Mn_(2)@N_(2),Cu_(2)@N_(1),and Ru_(2)@N_(3)endow the best catalytic activity with corresponding limiting potentials of-0.26,-0.18,-0.17,-0.39,and-0.30 V,re-spectively.Furthermore,on g-C_(3)N_(4)and graphdiyne,triple-atom sites(TAS,M_(3))such as Ru_(3)(Co_(3))@g-C_(3)N_(4)and Ru_(3)(Rh_(3))@graphdiyne are expected to exhibit higher stability and NRR catalytic performance than single-atom sites(SAS)and dual-atom sites(DAS),with corresponding limiting potentials of-0.28,-0.48,-0.24,and-0.23 V.The calculated results with the corresponding experimental potentials indicate that the origin of superior NRR ac-tivity observed in experiments may be contributed by M_(2)or M_(3)on 2D materials.This study provides an in-depth investigation into real active NRR sites of metal atoms supported on 2D materials and contributes to the design of effective NRR catalysts.
基金supported by NSFC(Grant No.52202265,52302004,52472010,62434010)the Taishan Scholars Program of Shandong Province(tsqn202306330)+1 种基金Shenzhen Science and Technology Program(JCYJ20230807094009018)Xiaomi Young Talents Program(2023XM06).
文摘Gallium nitride(GaN)single crystal with prominent electron mobility and heat resistance have great potential in the high temperature integrate electric power systems.However,the sluggish charge storage kinetics and inadequate energy densities are bottlenecks to its practical application.Herein,the self-supported GaN/Mn_(3)O_(4) integrated electrode is developed for both energy harvesting and storage under the high temperature environment.The experimental and theoretical calculations results reveal that such integrated structures with Mn-N heterointerface bring abundant active sites and reconstruct low-energy barrier channels for efficient charge transferring,reasonably optimizing the ions adsorption ability and strengthening the structural stability.Consequently,the assembled GaN based supercapacitors deliver the power density of 34.0 mW cm^(-2) with capacitance retention of 81.3%after 10000 cycles at 130℃.This work innovatively correlates the centimeter scale GaN single crystal with ideal theoretical capacity Mn_(3)O_(4) and provides an effective avenue for the follow-up energy storage applications of the wide bandgap semiconductor.
基金National Natural Science Foundation of China(No.22272149,22062025)Yunnan University’s Research Innovation Fund for Graduate Students(No.KC-23234085)+1 种基金Workstation of Academician Chen Jing of Yunnan Province(No.202105AF150012)Free Exploration Fund for Academician(No.202405AA350001)。
文摘Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high current densities.Herein,a Pr-doped Co(OH)_(2)hexagonal sheet(Pr/Co=1/9,in mole)is synthesized by electrodeposition as highly performant catalyst for 5-hydroxymethylfurfural(HMF)oxidation reaction(HMFOR)to produce 2,5-furandicarboxylic acid(FDCA).This novel and low-cost catalyst possesses a rather low onset potential of 1.05 V(vs.RHE)and requires only 1.10 V(vs.RHE)to reach a current density of 10 mA cm^(-2)for HMFOR,significantly outperforming Co(OH)_(2)benchmark(i.e.,210 mV higher to reach10 m A cm^(-2)).The origin of Pr promotion effect as well as the evolution of CoOOH catalytic sites and HMFOR process has been deeply elucidated by physical characterizations,kinetic experiments,in situ electrochemical techniques,and theoretical calculations.The unique Pr-ameliorated CoOOH active centers enable 100%conversion of HMF,99.6%selectivity of FDCA,and 99.7%Faraday efficiency,with a superior cycling durability toward HMFOR.This can be one of the most outstanding results for Co-based HMFOR catalysts to date in the literature.Thereby this work can help open up new horizons for constructing novel and efficient Co-based electrocatalysts by the utilization of lanthanide elements.
基金supported by the National Natural Science Foundation of China(No.21773089)the Henan Center for Outstanding Overseas Scientist(No.GZS2024004).
文摘Herein,a new type of two-dimensional(2D)/2D Ti_(3)C_(2)/TiO_(2) heterojunction was developed for efficient photocatalytic nitrogen reduction reaction(NRR),in which TiO_(2) nanosheets(TiO_(2) Ns)were designed as the main catalyst,while Ti_(3)C_(2) MXene served as the co-catalyst.Experimental and theoretical results revealed that Ti_(3)C_(2) MXene introduced electron-rich unsaturated Ti sites,serving as highly active sites for both the adsorption and activation of N_(2) on the Ti_(3)C_(2)/TiO_(2) heterojunction.Furthermore,the 2D/2D Ti_(3)C_(2)/TiO_(2) heterostructure greatly promoted the directional separation and transfer of charge carriers,facilitated by the internal electric field.This structural feature enabled the spatial separation of the N_(2) reduction and H2 O oxidation half-reactions on the distinct surfaces of Ti_(3)C_(2)(001)and TiO_(2)(001),con-sequently reducing the reaction energy barrier for each respective process.The synergistic effects arising from the interface and surface interactions within the heterojunction conspicuously improved the photo-catalytic NRR activity.As a result,the optimized Ti_(3)C_(2)/TiO_(2) heterojunction exhibited a high NH_(3) produc-tion rate of 24.4μmol g−1 h−1 in the absence of sacrificial agents,representing a remarkable 12.8-fold increase compared to individual TiO_(2) Ns.This work provides new insights into rational design of high-performance heterogeneous photocatalysts and offers a deeper understanding of the mechanism under-lying surface active sites in the photocatalytic NRR process.
基金supported by Research Grant from China Petroleum and Chemical Corp。
文摘Cu/ZnO-based catalysts are widely employed for methanol synthesis via CO_(2) hydrogenation.The preparation procedure is sensitive to the particle size and interfacial structure,which are considered as potential active centers influencing the rate of both methanol and CO formation.The particle size and the interaction between Cu and the support materials are influenced by the coprecipitation conditions,let alone that the mechanistic divergence remains unclear.In this work,a series of Cu/ZnO/ZrO_(2) catalysts were prepared via co-precipitation at different pH value and systematically characterized.The structure has been correlated with kinetic results to establish the structure-performance relationship.Kinetic analysis demonstrates that methanol synthesis follows a single-site Langmuir-Hinshelwood(L-H)mechanism,i.e.,Cu serves as the active site where CO_(2) and H_(2) competitively adsorb and react to form methanol.In contrast,CO formation proceeds via a dual-site L-H mechanism,where CO_(2) adsorbs onto ZnO and H_(2) onto Cu,with the reaction occurring at the Cu/ZnO interface.Therefore,for the direct formation of methanol,solely reducing the particle size of Cu would not be beneficial.
基金supported by the International Cooperation and Exchange Program of the National Natural Science Foundation of China(32261133531)。
文摘The kidney is essential for maintaining fluid,electrolyte,and metabolite homeostasis,and for regulating blood pressure.The pig serves as a valuable biomedical model for human renal physiology,offering insights across different physiological states.In this study,single-cell RNA sequencing was used to profile 138469 cells from 12 pig kidney samples collected during the embryonic(E),fattening(F),and pregnancy(P)periods,identifying 29 cell types.Proximal tubule(PT)cells exhibited elevated expression of metabolism-related transcription factors(TFs),including GPD1,ACAA1,and AGMAT,with validation across multiple individuals,periods,and species.Fluorescence homologous double-labeling of paraffin sections further confirmed the expression of ACAA1 and AGMAT in PT cells.Comparative analysis of pig and human kidneys revealed a high degree of similarity among corresponding cell types.Analysis of cell-type heterogeneity highlighted the diversity of thick ascending limb(TAL)cells,identifying a TAL subpopulation related to immune function.Additionally,the functional heterogeneity of kidney-resident macrophages(KRM)was explored across different anatomical sites.In the renal medulla,KRM were implicated in phagocytosis and leukocyte activation,whereas in the renal pelvis,they functioned as ligands,recruiting neutrophils with bactericidal activity to the renal pelvis to combat urinary tract infections.
基金supported by the Young Scientific and Technological Talents(Level Two)in Tianjin(No.QN20230214)Climbing Program of Tianjin University(No.2023XPD-0006)+1 种基金National Natural Science Foundation of China(No.52100156)National Engineering Research Center for Digital Construction and Evaluation Technology of Urban Rail Transit(No.2023HJ02)for the financial support。
文摘The type and quantity of active sites on a catalyst surface determine catalytic activity.In this study,machine learning was employed to assist in the construction of C=O and pyridine N active sites using sludge waste.Reactive descriptors,including C%,N%,O%,Fe%,pyrolysis temperature,heating rate,and pyrolysis time were proposed.Decision tree,extra tree,extreme gradient boosting(XGB),automatic relevance determination,and Bayesian ridge regression models were constructed and optimized.Among these,the XGB model was demonstrated with superior accuracy for prediction of C=O sites on the catalyst surface.Additionally,an ensemble model combining extra trees and XGB was developed to predict pyridine N,with R~2 value as high as 0.80 and minimum root mean square error(RMSE)of 0.1386.The ensemble model demonstrated a 17%improvement in accuracy compared to individual models.The model enables high-throughput screening of construction conditions for C=O and pyridine N.The study found that a pyrolysis temperature above of 500–800℃,a heating rate of 10–20℃/min,and a heating time of 120–200 min favor the generation of C=O active sites.For pyridine N sites,a pyrolysis temperature between 400℃ and 600℃,a heating rate of 5–10℃/min,and a pyrolysis time of around 150 min are optimal.Experimental validation demonstrated that both models exhibit excellent predictive performance,with prediction errors below 10%in all cases.This research provides a method to assist in the construction of C=O and pyridine N active sites,which is beneficial for guiding the design of sludge catalysts.
文摘In Lima(the capital of Peru),archaeological sites are constantly being threatened by accelerated urban expansion.This study examines Independencia(a district in northern Lima),where 95%of archaeological areas have been encroached upon due to inadequate planning and conservation policies.Focusing on four key archaeological sites(Cerro La Cruz,Cerro San Jerónimo,Pampa de Cueva,and San Jerónimo),this study employed a comprehensive pathological analysis to assess the extent and causes of deterioration.Data were gathered through field observation sheets based on the Ministry of Culture’s Conservation Guide,alongside historical photographs,aerial imagery,and urban mapping.The results indicate that human agents(27.1%)are the primary drivers of damage,supplemented by fortuitous(4.07%)and biological(2.89%)agents.The pronounced deterioration,particularly from human agents,underscores the urgent need for a holistic conservation strategy that integrates community participation with technical heritage management,ensuring that Lima’s pre-Hispanic legacy is preserved amidst ongoing urban pressure.
文摘Two protected sites located on the outskirts of the Sena Oura National Park (PNSO) in West Mayo-Kebbi cover an area of 1800 m2 is pattern choose in pastoral enclave in both village. This study was undertaken to highlight the floristic diversity of the herbaceous and woody vegetation on these sites in the offing to know the ability of charge into UBT that most support the park peripheral. It took place on two experimental sites on a natural course in two villages: Wazetelan and Massang. The approach used for the study was a survey using the systematic sampling method and a 30 m × 30 m plot. The survey consisted in listing all the taxa in a floristically homogeneous plot, each assigned the Braun-Blanquet dominance abundance coefficient. These surveys revealed a floristic richness of 73 species, 58 genera, including 46 herbaceous and 26 woody species. The Shannon result gives H1' = 0.12 bit for herbaceous species and H2' = 0.44 bit for woody species, meaning that the herbaceous and woody populations of all the surveys have a very low species diversity, as H' < 3 according to the Shannon index assessment threshold. Herbaceous species are divided into 13 families and 33 genera. The most represented families are Fabaceae (27.3%) and Poaceae (21.9%). Most of the other families (1.3%) have only one species, if any. Herbaceous species are divided into 33 genera grouped into 13 families. The most represented families are Fabaces (16 species), 34%, and Poaceae (12 species), 26%. The 26 woody species, most of which come from itinerant surveys, are distributed across 24 genera and 12 families, the most important of which is Fabaceae with 09 species (34.6%). This floristic assessment, in terms of quantity and quality, has enabled us to estimate the carrying capacity of the two pastoral enclaves in Dari and Goumadji cantons, and to guide the government’s actions with regard to rangeland management.
文摘As an important pillar of China's industrialization process,the coal industry has not only made contributions to economic growth,but also left a large number of coal mine sites bearing historical memories.These sites are not only the witness of the industrial civilization,but also the potential resources for urban renewal and industrial transformation.
基金supported by the Natural Science Foundation of Shandong Province (ZR2024JQ004)the National Natural Science Foundation of China (22108306, 22478432)Taishan Scholars Program of Shandong Province
文摘Disrupting the symmetric electron distribution of porphyrin-like Fe singleatom catalysts has been considered as an effective way to harvest high intrinsic activity.Understanding the catalytic performance governed by geometric microstrains is highly desirable for further optimization of such efficient sites.Here,we decipher the crucial role of local microstrain in boosting intrinsic activity and durability of asymmetric Fe single-atom catalysts(Fe-N_(3)S_(1))by replacing one N atom with S atom.The high-curvature hollow carbon nanosphere substrate introduces 1.3%local compressive strain to Fe-N bonds and 1.5%tensile strain to Fe-S bonds,downshifting the d-band center and accelerating the kinetics of*OH reduction.Consequently,highly curved Fe-N_(3)S_(1)sites anchored on hollow carbon nanosphere(FeNS-HNS-20)exhibit negligible current loss,a high half-wave potential of 0.922 V vs.RHE and turnover frequency of 6.2 e^(−1)s^(−1)site−1,which are 53 mV more positive and 1.7 times that of flat Fe-N-S counterpart,respectively.More importantly,multiple operando spectroscopies monitored the dynamic optimization of strained Fe-N_(3)S_(1)sites into Fe-N_(3)sites,further mitigating the overadsorption of*OH intermediates.This work not only sheds new light on local microstrain-induced catalytic enhancement,but also provides a plausible direction for optimizing efficient asymmetric sites via geometric configurations.
基金supported by the National Natural Science Foundation of China(Nos.22076098,22376118 and 21577078)the Outstanding Youth Project of the Natural Science Foundation of Hubei Province(2023AFA054)the 111 Project of China(No.D20015).
文摘Enhancing the catalytic hydrolysis efficiency of microcystins(MCs)at ambient temperature has been a persistent challenge in water treatment.We employed N_(2)/low-temperature plasma technology to modify the surface of natural pyrites(NP),and the resulting nitrogenmodified pyrites(NPN)with a nanorod structure and new Fe-Nx sites are more efficient for the hydrolysis of microcystins-LR(MC-LR).Kinetic experiments revealed that NPN exhibited significantly higher hydrolysis activity(k_(obs)=0.1471 h^(-1))than NP(0.0914 h^(-1)).Liquid chromatography-mass spectrometry(LC/MS)for the intermediates produced by hydrolyzing MC-LR,in situ attenuated total reflectance Fourier transform infrared spectroscopy(in situ ATR-FTIR)and X-ray photoelectron spectroscopy(XPS)analysis unfolded that the Fe and N atoms of Fe-Nx sites on the surface act of NPN as Lewis acid and Bronsted basic respectively,selectively breaking amide bond on MC-LR molecule.This study demonstrates the effectiveness of plasma technology in modifying mineral materials to enhance their catalytic activity,providing a new method for eliminating MCs in practical water treatment.
基金supported by the National Natural Science Foundation of China(Nos.U22A20402,U21A20286,and 22102100)the Key Program of Shenzhen Science and Technology Commission(No.JCYJ20220818095601002)the Natural Science Foundation of Shanghai(No.22ZR1431700).
文摘Atomic hydrogen(H∗)plays a crucial role in electrochemical reduction technology towards various environmental and energy applications,but suffers from low utilization efficiency arisen from the undesirable H-H dimerization and the competitive adsorption between water molecule with reactants on the traditional adjacent catalytic sites.Herein,we anchored Pd single atoms on the naturally formed titanium oxide of titanium foam to construct Pd_(1)-O-Ti dual-site electrocatalyst with spatially isolated water dissociation and H∗utilization site,which synchronously inhibits the H-H dimerization and the competitive adsorption of water molecule and targeted reactants.Experiments and theoretical calculations revealed that the Ti-O sites could synergistically dissociate water to H∗,which overflowed to nearby Pd single-atom sites for designed reduction reactions and utilization benefiting from the hydrogen spillover ability of titanium oxide substrate.These Pd_(1)-O-Ti dual sites delivered almost 100%bromate reduction efficiency with a rate constant of 1.57 h^(-1),far superior to those of Pdn-O-Ti with adjacent Pd sites(0.52 h^(-1)),Pd_(1)-N-C with single sites(0.04 h^(-1))and commercial Pd/C(0.18 h^(-1)),respectively.This study sheds light on the importance of integrating synergistic active sites for complicated electrochemical reactions,and provide new insights in improving H∗ utilization for environmental remediation.
基金supported by the National Natural Science Foundation of China(Nos.52408435,52278384)。
文摘Ground response analysis and determination of site-specific ground motion parameters are necessary for evaluating seismic loads to enable sustainable design of aboveground and underground structures,particularly in deep overburden sites.This study investigates the influence of bedrock interface conditions and depth of soil deposits on obtained site-specific ground motion parameters.Employing the one-dimensional seismic response analysis program SOILQUAKE,the ground responses of five representative soil profiles and 1050 case studies are calculated considering three different site models of seismic input interfaces.The analysis employs the actual bedrock interface with a shear wave velocity of 760 m/s as the reference input bedrock interface.The results illustrate that the selection of the bedrock interface condition significantly affects the seismic response on the ground surface of deep overburden sites.Specifically,the ground surface acceleration response spectra at longer periods are notably smaller compared to those at the actual bedrock site.This may present a challenge for designing long-period high-rise buildings situated in deep overburden sites.It is recommended to select a seismic input bedrock interface closely approximating the actual bedrock depth when conducting seismic response analyses for deep overburden sites.
基金National Natural Science Foundation of China(No.22005154)for financial support。
文摘Photocatalytic CO_(2)reduction reaction(CO_(2)RR)is one of the promising strategies for sustainably producing solar fuels.The precise identification of catalytic sites and the enhancement of photocatalytic CO_(2)conversion is imperative yet quite challenging.This critical review summarizes recent advances in porous photo-responsive polymers,including covalent organic frameworks(COFs),covalent triazine frameworks(CTFs),and conjugated microporous polymers(CMPs),those can be rationally designed from the molecular level for visible-light-driven photocatalytic CO_(2)reduction.Additionally,special emphasis is placed on how the well-defined active sites on these polymers can influence their properties and photocatalytic performance.The precise regulation and control of microenvironments and electronic properties of metal active centers are crucial for boosting catalytic efficiency and selectivity,as well as for the design of better photocatalysts for CO_(2)reduction.
