Distinguishing the main components of submarine groundwater and estimating the corresponding fluxes based on radium tracing method—taking the Maowei Sea for example

Submarine groundwater discharge(SGD)is an important part in the land-sea interactions,which mainly contains three components:submarine fresh groundwater discharge(SFGD),tidal flat recirculated saline groundwater discharge(tidal flat RSGD)and subtidal recirculated saline groundwater discharge(subtidal RSGD).In order to make a more accurate assessment of the impact of SGD on coastal ecological environment,it is necessary to distinguish the main components of SGD.In this study,the Maowei Sea,located in the northern part of the Beibu Gulf,was selected as the study area.Based on the radium(Ra)tracing method,we present a new analytical method for distinguishing the three main components of SGD in this area combined with field data.The average daily flow along the coastline of the Maowei Sea of tidal flat RSGD was slightly higher than that of SFGD,and both two were on the magnitude of 1×10^(5)m^(3)/d.The average daily flow for the subtidal RSGD of the entire subtidal zone of the Maowei Sea reached to the magnitude of 1×10^(6)-1×10^(7)m^(3)/d.The long-term variation trend of terrestrial SGD is a valuable information for the study of the influence of terrigenous material on the coastal ecological environment.Based on the results of four sampling periods,it is found that the fluxes of SFGD and tidal flat RSGD in the Maowei Sea had good linear correlation with the net precipitation.As an example,January 2015 to August 2022 were selected as the study periods,and the variation trends of SFGD and tidal flat RSGD were calculated by linear function with net precipitation as the independent variable.The results showed that the flux of tidal flat RSGD was slightly higher than that of SFGD,and the difference between the two is larger in flood season while smaller in dry season.In general,in the coastal range of China,the total SGD flux in the Maowei Sea area is at a high level,and the SFGD flux is at a medium level.

Ⅰ期非小细胞肺癌达芬奇机器人手术的疗效分析

背景与目的达芬奇机器人手术系统在胸外科的应用日益广泛,本研究旨在探讨经达芬奇机器人手术治疗I期非小细胞肺癌(non-small cell lung cancer, NSCLC)患者的疗效。方法回顾2012年1月-2017年12月于我科行手术治疗的Ⅰ期NSCLC患者347例,依据手术方式分为机器人(robot-assisted thoracic surgery, RATS)组134例及腔镜(videoassisted thoracic surgery, VATS)组213例。比较两组患者围术期一般指标(术中出血量、术后引流量、术后带管时间、术后住院时间、淋巴结清扫状况),分析患者生存状况(overall survival, OS)、无进展生存状况(disease free survival, DFS)及相关影响因子。结果机器人组与腔镜组术中出血量[(49±39) mL vs (202±239) mL]、术后引流量[Day 1:(248±123)mL vs (350±213) mL; Day 2:(288±189) mL vs (338±189) mL]比较,机器人组均少于腔镜组(P<0.05);术后带管时间[(10±5) d vs (11±8) d]及住院时间[(13±6) d vs (14±9) d]两组患者无明显差异(P>0.05)。机器人组与腔镜组的淋巴结清扫组数[(5±2)组vs (4±2)组]及淋巴清扫数量[(18±9)枚vs(11±8)枚]比较,机器人组均优于腔镜组(P<0.05)。机器人组与腔镜组生存状况比较[1年生存率:97.3%vs 96%、3年生存率:89.8%vs 83.1%、5年生存率:87.5%vs 70.3%,平均生存时间(month):61 vs 59],两组无统计学差异(P>0.05)。无进展生存状况:机器人组与腔镜组比较[1年无进展生存率:93.7%vs 91.3%、3年无进展生存率:87.7%vs 68.4%、5年无进展生存率:87.7%vs 52.5%,平均无进展生存时间(month):61 vs 50],机器人组明显优于腔镜组(P<0.05)。单因素分析显示,淋巴结清扫数量是患者生存状况的影响因子;肿瘤直径、手术方式、淋巴结清扫组数、淋巴结清扫数量为患者无进展生存状况的影响因子。多因素分析显示生存状况无独立影响因子,肿瘤直径及手术方式为无进展生存状况的独立影响因子。结论达芬奇机器人Ⅰ期非小细胞肺癌患者术后生存状况与腔镜手术无差异,但无进展生存状况优于腔镜手术;达芬奇机器人手术淋巴结清扫更彻底,同时术中出血量更少。

铁诱导生长在碳布上三维纳米多孔铁钴羟基氧化物作为高效电催化析氧反应电极（英文）

开发高效、廉价的电极材料应用于电催化氧析出反应(OER)在水分解技术中起着至关重要的作用.提高催化剂催化活性的策略主要有两种,一是通过调整催化剂形貌和结构来增加催化活性位点数量,二是通过掺入其它组分来增强催化活性位点的反应活性.本工作结合这两种策略,通过原位电氧化方法成功合成了生长在碳布上具有独特三维结构的纳米多孔铁钴羟基氧化物(3D-FeCoOOH/CC),合成的电极材料直接用作电催化析氧反应的工作电极.以生长在碳布上的“微型棋子”阵列(MCPAs/CC)作为前驱体,先后通过在(NH4)2Fe(SO4)2溶液中进行Fe掺杂工艺和在碱性介质中原位电化学氧化制备了3D-FeCoOOH/CC.微观表征表明,MCPAs/CC上的“微型棋子”阵列完全转化为一层薄形涂层包覆在碳布纤维上.电化学测试结果表明,合成的3D-FeCoOOH/CC在1.0 mol L^-1 KOH溶液中表现出优异的OER催化活性,在电流密度为10 mA cm^-2时所需的过电势仅为259 mV,塔菲尔斜率为34.9 mV dec^-1,并且具有优异的稳定性.详细的表征表明,电化学表面积的增加、电导率的增高、FeCo双金属组成和独特的3D多孔结构共同使得3D-FeCoOOH/CC的催化OER活性增强.此外,本实验所应用的合成策略可以扩展到制备一系列其他过渡元素掺杂的Co基电极材料.利用选区电子衍射、红外光谱和XPS等技术证明了双金属羟基氧化物的合成.从扫描电子显微镜图和透射电子显微镜图可以看出,本实验所合成的3D-FeCoOOH/CC具有多孔结构,相应的元素分布图表明Fe和Co元素在催化剂中均匀分布.N2吸脱附测试进一步证明了多孔结构的生成.XPS测试结果表明,前驱体中Co元素为+2价,3D-CoOOH/CC中的Co元素为+3价,Co 2p电子结合能分别为780.5和795.7 eV,当将Fe引入其中时,3D-FeCoOOH/CC中的Co元素也为+3价,但Co 2p电子结合能变为780.9和796.1 eV.相比于3D-CoOOH/CC,3D-FeCoOOH/CC中Co元素的电子结合能增加了0.4 eV,这表明Fe的引入调节了Co原子的电子结构,并且Fe原子和Co原子之间存在强烈的相互作用.3D-FeCoOOH/CC在~785 eV处增强的Co的伴随峰表明Co原子的简并轨道被破坏引起Co 3d电子群重排,而Co 3d电子群的重排导致Co原子电子密度增加,有利于催化活性的增强.此外Fe元素的加入可以调节OH在催化剂上的吸附,从而增强催化活性.3D-FeCoOOH/CC表现出优异的电催化析氧性能,可以归因于以下几方面:首先,Fe元素掺入提高电极材料的电化学活性面积(ECSA)、电导率和质量传递;其次,Co与掺杂Fe之间的强烈相互作用调节了电子密度和OH在催化剂表面吸附;第三,3D-FeCoOOH/CC独特的3D多孔结构具有较大的表面积,有利于催化活性位点的暴露、电解质与催化剂的接触和产生氧气的释放;第四,独特的3D多孔电极材料具有良好的结构稳定性,从而使3D-FeCoOOH/CC具有更好的稳定性.得益于上述优势,本实验所合成的3D-FeCoOOH/CC电极表现出优异的电催化析氧性能.

Estimating submarine groundwater discharge at a subtropical river estuary along the Beibu Gulf,China

In certain regions,submarine groundwater discharge(SGD)into the ocean plays a significant role in coastal material fluxes and their biogeochemical cycle;therefore,the impact of SGD on the ecosystem cannot be ignored.In this study,SGD was estimated using naturally occurring radium isotopes(^(223)Ra and ^(224)Ra)in a subtropical estuary along the Beibu Gulf,China.The results showed that the Ra activities of submarine groundwater were approximately 10 times higher than those of surface water.By assuming a steady state and using an Ra mass balance model,the SGD flux in May 2018 was estimated to be 5.98×10^(6) m^(3)/d and 3.60×10^(6) m^(3)/d based on 224Ra and 223Ra,respectively.At the same time,the activities of Ra isotopes fluctuated within a tidal cycle;that is,a lower activity was observed at high tide and a higher activity was seen at low tide.Based on these variations,the average tidal pumping fluxes of SGD were 1.15×10^(6) m^(3)/d and 2.44×10^(6) m^(3)/d with 224Ra and 223Ra,respectively.Tidaldriven SGD accounts for 24%-51%of the total SGD.Therefore,tidal pumping is an important driving force of the SGD in the Dafengjiang River(DFJR)Estuary.Furthermore,the SGD of the DFJR Estuary in the coastal zone contributes significantly to the seawater composition of the Beibu Gulf and the material exchange between land and sea.

Pt-confinement catalyst with dendritic hierarchical pores on excellent sulfur-resistance for hydrodesulfurization of dibenzothiophene and 4,6-dimethyldibenzothiophene

Metal confinement catalyst Mo S_(2)/Pt@TD-6%Ti(TD,TS-1/Dendritic mesoporous silica nanoparticles composite) in dendritic hierarchical pore structures was synthesized and showed excellent sulfur-resistance performance and stabilities in catalytic hydrodesulfurization reactions of probe sulfide molecules.The Mo S_(2)/Pt@TD-6%Ti catalyst combines the concepts of Pt-confinement effect and hydrogen spillover of Pt noble metal.The modified micropores of Mo/Pt@TD-6%Ti only allow the migration and dissociation of small H_(2) molecules(0.289 nm),and effectively keep the sulfur-containing compounds(e.g.H_(2)S,0.362 nm) outside.Thus,the Mo S_(2)/Pt@TD-6%Ti catalyst exhibits higher DBT and 4,6-DMDBT HDS activities because of the synergistic effect of the strong H_(2) dissociation ability of Pt and desulfurization ability of Mo S_(2) with a lower catalyst cost.This new concept combining H2dissociation performance of noble metal catalyst with the desulfurization ability of transition metal sulfide Mo S_(2) can protect the noble metal catalyst avoiding deactivation and poison,and finally guarantee the higher activities for DBT and 4,6-DMDBT HDS.

Perspective on powder technology for all-solid-state batteries:How to pair sulfide electrolyte with high-voltage cathode

Sulfide solid electrolytes(SEs)have attracted ever-increasing attention due to their superior roomtemperature ionic conductivity(~10^(-2) S cm^(-1)).Additionally,the integration of sulfide SEs and highvoltage cathodes is promising to achieve higher energy density.However,the incompatible interfaces between sulfide SEs and high-voltage cathodes have been one of the key factors limiting their applications.Therefore,this review presents a critical summarization of the interfacial issues in all-solid-state lithium batteries based on sulfide SEs and high-voltage cathodes and proposes strategies to stabilize the electrolyte/cathode interfaces.Moreover,the future research direction of electrolyte/cathode interfaces and application prospects of powder technology in sulfide-based ASSLBs were also discussed.

The impact of China’s high-speed rail investment on regional economy and air pollution emissions

The high-speed rail(HSR)network in China has experienced rapid development since the 2000s.In 2016,the State Council of the People’s Republic of China issued a revised version of the“Mid-and Long-term Railway Network Plan”,detailing the expansion of the railway network and construction of an HSR system.In the future,the HSR construction efforts in China will further increase,which is considered to impact regional development and air pollutant emissions.Therefore,in this paper,we apply a transportation network-multiregional computable general equilibrium(CGE)model to estimate the dynamic effects of HSR projects on economic growth,regional disparities,and air pollutant emissions in China.The results indicate that HSR system improvement could generate a positive economic impact but could also increase emissions.The gross domestic product(GDP)growth per unit investment cost stimulated by HSR investment is found to be the largest in eastern China but the smallest in the northwest regions.Conversely,HSR investment in Northwest China contributes to a substantial reduction in regional disparities in terms of the GDP per capita.In regard to air pollution emissions,HSR construction in South-Central China results in the largest increase in CO_(2) and NO_(X) emissions,while for CO,SO_(2),and fine particulate matter(PM_(2.5))emissions,the largest increase occurs due to HSR construction in Northwest China.At the regional level,the provinces with large changes in accessibility also experience large changes in their air pollutant emissions.

Inherently Chiral 6,7-Diphenyldibenzo [e,g][1,4]diazocine: Enantioselective Synthesis and Application as a Ligand Platform

Inherently chiral 6,7-diphenyldibenzo[e,g][1,4]diazocine(DDD)has been synthesized enantioselectively for the first time via chiral phosphoric acid(CPA)-catalyzed cyclocondensation of readily available[1,1′-biphenyl]-2,2′-diamine(1a)and benzil(2a)in 82%yield,with 98%ee under mild reaction conditions.The strategy could also be applied to racemic biaryl diamines through kinetic resolution.The unexpectedly high interconversion energy barriers between the enantiomers(ΔG=39.5 kcal/mol)and the chemical stability rendered DDD an ideal platform for developing new chiral ligands and catalysts.Unique inherently chiralDDD-based phosphoramidites,phosphoric acid,mono-and diphosphine ligands were prepared from optically pure diphenol derivative DDDOL as a common precursor.Preliminary asymmetric reactions catalyzed by Pd or Rh in the presence of newly developed ligands exhibited comparable or even better enantioselectivities than the corresponding BINOLor SPINOL-derived ligands.Density functional theory calculation revealed the origin of the enantioselectivity during the process.

利用昆虫携带的花粉初探西藏入侵植物印加孔雀草在当地传粉网络中的地位

入侵植物在新生境中成功定殖后,通过利用当地传粉昆虫促进繁殖可以更好地保证种群的扩张,但是入侵植物在当地传粉网络中的角色和地位仍不是很清楚。本文利用西藏近年发现的入侵植物印加孔雀草(Tagetes minuta),分析其访花昆虫所携带的植物花粉种类,构建了植物花粉–传粉者网络,探讨印加孔雀草快速入侵和扩张的可能机制。结果表明印加孔雀草为泛化传粉系统,共有13种昆虫访花,其中12种携带有印加孔雀草花粉,所有花粉中印加孔雀草花粉数量占比为89.89%。12种印加孔雀草传粉昆虫中, 4种泛化传粉昆虫(1种蜂、2种食蚜蝇和1种蝇)是其主要传粉昆虫。本研究揭示印加孔雀草在较短时间内已经成功利用多种当地泛化传粉昆虫为其授粉,已顺利融入当地的传粉网络,今后需要更加重视对印加孔雀草的防控。

Primer Extension Reaction Assays for Incorporation of Deoxynucleotide Analogue into DNA

Incorporation of deoxynucleotide analogues into DNA is important for the expansion of DNA functions.Primer extension reactions are commonly used for the assay of such reaction events.However,current assay protocols generally rely on radiolabeling,fluorescence reporter labeling,or removal of specific deoxynucleotide triphosphate in the reaction mixture.Herein we report on the design of two novel assay protocols that utilize a dideoxynucleo-tide-terminated template strand and a phosphorothiolate-modified deoxynucleotide-terminated template strand.We designed and synthesized a deoxyuridine triphosphate analogue(dU^(*)TP)containing 2-bromoisobutyryl group and demonstrated that it could be well recognized byφ29DNA polymerase,E.coli DNA polymerase I Klenow Fragment,Bst DNA polymerase Large Fragment,and E.coli DNA polymerase I Klenow Fragment(exo^(−)),which translated to effective incorporation of dU^(*)TP into DNA.dU^(*)TP was also successfully incorporated into extremely long single-stranded DNA at high-density usingφ29 DNA polymerase by rolling circle amplification.

A New Saddle-Shaped Aza Analog of Tetraphenylene: Atroposelective Synthesis and Application as a Chiral Acylating Reagent

(Z)-7-Aryl-5-acyldibenzo[e,g][1,4]diazocin-6(5H)-one,a unique saddle-shaped bridged biaryl containing synchronized aryl–aryl and N-aryl stereogenic axes,was constructed for the first time in good yields with up to 96%enantiomeric excess(ee).The threecomponent coupling reaction,involving aryl iodide,2,2′-diisocyano-1,1′-biphenyl,and carboxylate,constructs the eight-membered ring in an atroposelective manner through palladium-catalyzed double isocyanide insertion followed by C–Obond formation during reductive elimination and amide formation after acyl transfer.

A2Str: Molecular Graph Generation Based on Given Atoms

Molecular graph generation is an emerging area of research withnumerous applications. Most existing approaches generate new molecules bylearning a generative model from a collection of known molecules. However,how to obtain the molecular structure from its atomic composition is a problemto be solved. In this paper, it proposes an autoencoder-based model called A2Strwhich takes the atomic composition of a molecular as input. Its molecular structurewas generated and model structures were designed. The effects were verified oneby one. In addition, experiments were implemented with isomer generation anddetermined that the ratio of more than 3% of molecules with different structurescan be obtained from the same combination of atoms.