Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a...Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.展开更多
Within the context of the Belt and Road Initiative(BRI)and the China-Myanmar Economic Corridor(CMEC),the Dulong-Ir-rawaddy(Ayeyarwady)River,an international river among China,India and Myanmar,plays a significant role...Within the context of the Belt and Road Initiative(BRI)and the China-Myanmar Economic Corridor(CMEC),the Dulong-Ir-rawaddy(Ayeyarwady)River,an international river among China,India and Myanmar,plays a significant role as both a valuable hydro-power resource and an essential ecological passageway.However,the water resources and security exhibit a high degree of vulnerabil-ity to climate change impacts.This research evaluates climate impacts on the hydrology of the Dulong-Irrawaddy River Basin(DIRB)by using a physical-based hydrologic model.We crafted future climate scenarios using the three latest global climate models(GCMs)from Coupled Model Intercomparison Project 6(CMIP6)under two shared socioeconomic pathways(SSP2-4.5 and SSP5-8.5)for the near(2025-2049),mid(2050-2074),and far future(2075-2099).The regional model using MIKE SHE based on historical hydrologic processes was developed to further project future streamflow,demonstrating reliable performance in streamflow simulations with a val-idation Nash-Sutcliffe Efficiency(NSE)of 0.72.Results showed that climate change projections showed increases in the annual precip-itation and potential evapotranspiration(PET),with precipitation increasing by 11.3%and 26.1%,and PET increasing by 3.2%and 4.9%,respectively,by the end of the century under SSP2-4.5 and SSP5-8.5.These changes are projected to result in increased annual streamflow at all stations,notably at the basin’s outlet(Pyay station)compared to the baseline period(with an increase of 16.1%and 37.0%at the end of the 21st century under SSP2-4.5 and SSP5-8.5,respectively).Seasonal analysis for Pyay station forecasts an in-crease in dry-season streamflow by 31.3%-48.9%and 22.5%-76.3%under SSP2-4.5 and SSP5-8.5,respectively,and an increase in wet-season streamflow by 5.8%-12.6%and 2.8%-33.3%,respectively.Moreover,the magnitude and frequency of flood events are pre-dicted to escalate,potentially impacting hydropower production and food security significantly.This research outlines the hydrological response to future climate change during the 21st century and offers a scientific basis for the water resource management strategies by decision-makers.展开更多
Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C couplin...Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C coupling as well as the competing hydrogen evolution reaction(HER) largely limit the efficiency for C_(2+)production in CORR. Here we report an overturn on the Faradaic efficiency of CORR from being HER-dominant to C_(2+)formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like Cu catalyst via pressuring CO. With the CO pressure rising from 1 to 40 atm, the C_(2+)Faradaic efficiency and partial current density remarkably increase from 22.8%and 18.9 mA cm^(-2)to 89.7% and 116.7 mA cm^(-2), respectively. Experimental and theoretical investigations reveal that high pressure-induced high CO coverage on metallic Cu surface weakens the Cu–C bond via reducing electron transfer from Cu to adsorbed CO and restrains hydrogen adsorption, which significantly facilitates the C–C coupling while suppressing HER on the predominant Cu(111) surface, thereby boosting the CO electroreduction to C_(2+)activity.展开更多
基金the National Natural Science Foundation of China(51303083)the National Natural Science Foundation of China for Excellent Young Scholars(51922050)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20191293)the Fundamental Research Funds for the Central Universities(30920021123)。
文摘Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.
基金Under the auspices of the Yunnan Scientist Workstation on International River Research of Daming He(No.KXJGZS-2019-005)National Natural Science Foundation of China(No.42201040)+1 种基金National Key Research and Development Project of China(No.2016YFA0601601)China Postdoctoral Science Foundation(No.2023M733006)。
文摘Within the context of the Belt and Road Initiative(BRI)and the China-Myanmar Economic Corridor(CMEC),the Dulong-Ir-rawaddy(Ayeyarwady)River,an international river among China,India and Myanmar,plays a significant role as both a valuable hydro-power resource and an essential ecological passageway.However,the water resources and security exhibit a high degree of vulnerabil-ity to climate change impacts.This research evaluates climate impacts on the hydrology of the Dulong-Irrawaddy River Basin(DIRB)by using a physical-based hydrologic model.We crafted future climate scenarios using the three latest global climate models(GCMs)from Coupled Model Intercomparison Project 6(CMIP6)under two shared socioeconomic pathways(SSP2-4.5 and SSP5-8.5)for the near(2025-2049),mid(2050-2074),and far future(2075-2099).The regional model using MIKE SHE based on historical hydrologic processes was developed to further project future streamflow,demonstrating reliable performance in streamflow simulations with a val-idation Nash-Sutcliffe Efficiency(NSE)of 0.72.Results showed that climate change projections showed increases in the annual precip-itation and potential evapotranspiration(PET),with precipitation increasing by 11.3%and 26.1%,and PET increasing by 3.2%and 4.9%,respectively,by the end of the century under SSP2-4.5 and SSP5-8.5.These changes are projected to result in increased annual streamflow at all stations,notably at the basin’s outlet(Pyay station)compared to the baseline period(with an increase of 16.1%and 37.0%at the end of the 21st century under SSP2-4.5 and SSP5-8.5,respectively).Seasonal analysis for Pyay station forecasts an in-crease in dry-season streamflow by 31.3%-48.9%and 22.5%-76.3%under SSP2-4.5 and SSP5-8.5,respectively,and an increase in wet-season streamflow by 5.8%-12.6%and 2.8%-33.3%,respectively.Moreover,the magnitude and frequency of flood events are pre-dicted to escalate,potentially impacting hydropower production and food security significantly.This research outlines the hydrological response to future climate change during the 21st century and offers a scientific basis for the water resource management strategies by decision-makers.
基金financial support from the National Key R&D Program of China (Nos. 2022YFA1504500, 2022YFA1503100)the National Natural Science Foundation of China (Nos. 21988101, 21890753, 22225204, 92145301, 22002160 and 22272174)+4 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB36030200)the CAS Project for Young Scientists in Basic Research (No. YSBR-028)the Fundamental Research Funds for the Central Universities (No. 20720220008)the Dalian National Lab for Clean Energy (DNL Cooperation Fund 202001)the Innovation Research Fund Project of DICP (No. DICP I202016)。
文摘Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C coupling as well as the competing hydrogen evolution reaction(HER) largely limit the efficiency for C_(2+)production in CORR. Here we report an overturn on the Faradaic efficiency of CORR from being HER-dominant to C_(2+)formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like Cu catalyst via pressuring CO. With the CO pressure rising from 1 to 40 atm, the C_(2+)Faradaic efficiency and partial current density remarkably increase from 22.8%and 18.9 mA cm^(-2)to 89.7% and 116.7 mA cm^(-2), respectively. Experimental and theoretical investigations reveal that high pressure-induced high CO coverage on metallic Cu surface weakens the Cu–C bond via reducing electron transfer from Cu to adsorbed CO and restrains hydrogen adsorption, which significantly facilitates the C–C coupling while suppressing HER on the predominant Cu(111) surface, thereby boosting the CO electroreduction to C_(2+)activity.
文摘目的分析体质量指数(Body mass index,BMI)与老年慢性心力衰竭(Chronic heart failure,CHF)患者血浆胱抑素C(cystatinC,Cys-C)、N末端B型利钠肽原(N-terminal pro-B-type natriuretic peptide,NT-proBNP)水平相关性,并分析血浆Cys-C、NT-proBNP评估老年CHF患者预后价值。方法选择2021年7月—2022年10月在本院接受治疗的192例老年慢性心力衰竭(CHF)患者作为研究对象,按照BMI指数分为肥胖组(49例)、超重组(68例)和正常组(75例)三组。对比各亚组患者血浆Cys-C、NT-proBNP水平差异,采用Pearson相关性分析的方式探究老年CHF患者BMI指数与血浆Cys-C、NT-proBNP相关性,对入组患者实施12个月随访,将患者按照预后情况区分为死亡组和存活组,对比两亚组患者血浆Cys-C、NT-proBNP水平差异并评估预后评估价值。结果肥胖组患者血浆Cys-C、NT-proBNP水平高于超重组,超重组患者血浆Cys-C、NT-proBNP水平高于正常组,差异具有统计学意义(P<0.05);入组老年CHF患者的BMI指数与其血浆Cys-C、NT-proBN水平均呈现明显的正相关性(r=0.7104,P<0.0001)(r=0.6603,P<0.0001);随访12个月显示,死亡组患者的血浆Cys-C、NT-proBNP水平显著高于存活组患者,差异具有统计学意义(P<0.05);血浆Cys-C、NT-proBNP对老年CHF预后评估曲线下面积(area under curv,AUC)为0.6930(P=0.0009)、0.7982(P<0.0001)。结论老年CHF患者随BMI指数升高,血浆Cys-C、NT-proBNP水平逐渐升高,血浆Cys-C、NT-proBNP对老年CHF临床结局具有一定的预测价值,进一步研究有推广应用于老年CHF预后评估潜力。
