A Case Study of Typical Regional Pollution Transport in Fuzhou City

Based on data of PM2.5 hourly concentration and HYSPLIT model backward trajectory in coastal cities of Fujian Province during January 25 -26, 2014, a typical regional pollution process affecting Fujian from the north to the south and the east to the west on January 26 was investiga- ted. Taking Fuzhou as an example, based on weather situation on the ground and at high altitudes as well as corresponding meteorological data such as wind direction, wind velocity, and visibility, the changes of meteorological elements before, during and after the pollution were compared. Based on the V-3θ atmospheric vertical structure diagrams, the weather reasons for the generation, maintaining and dissipation of the pollution were discussed. The results indicated that the regional pollution was transported from the northeast to the southwest. The northeasterly air flow in front of the cold ridge strengthened and moved toward the east, so that the pollutant from the north affected Fujian form the north to the south and from the east to the west. As a result, there was a dramatic increase of pollutant concentration, rapid drop of visibility, and deterioration of air quality in the affected areas. The heavy pollution process featured high-speed transport and short-time generation. The air quality changed from good state to heavy pollution in just 3 -4 hours. The maximum of IAQIpM2.5 reached 280. The whole pollution process lasted for 14 hours. Solar radiation had been deeply affected by aerosol clouds, so that atmospheric stratification was extremely stable. Along with the eastward movement of cold high pressure into the sea, the dominant wind direction near the ground changed from the northeast to the east, so that the source of the pollutant was cut off , and air quality quickly turned well. The changes of atmospheric vertical structure indicated that the high inversion layer and clouds near 700 hPa kept lower air clean and blocked upper pollution transport. The later sudden increase of wind speed and strengthening of atmospheric mechanical turbu- lent destroyed inversion layer, so that the upper pollutants invaded air near the ground rapidly. During the period of high pollution, the isothermal layer （aerosol clouds） leaded to decrease of wind speed, and the atmosphere became more stable. The pollution ended until the wind field changed.

De novo assembly of chloroplast genomes of Corchorus capsularis and C.olitorius yields species-specific InDel markers

Jute(Corchorus spp.)is a member of the Malvaceae family,which comprises more than 100 species.The systematic positions of jute species have remained unsettled.Chloroplasts are maternally inherited and their genomes are widely used for plant phylogenetic studies.In the present study,the chloroplast genomes of Corchorus capsularis and C.olitorius were assembled,with sizes of respectively 161,088 and 161,766 bp.Both genomes contained 112 unique genes(78 protein-coding,four rRNA,and 30 tRNA genes).Four regionswith high variation between the two species were located in single-copy rather than inverted-repeat regions.A total of 66 simple sequence repeats(SSRs)were identified in the C.capsularis chloroplast genome and 56 in that of C.olitorius.Comparison of the two chloroplast genome sequences permitted the evaluation of nucleotide variation including 2417 single-nucleotide polymorphisms sites and 294 insertion or deletion sites,of which one marker(cpInDel 205)could discriminate the two jute species.Comparison of the C.capsularis and C.olitorius chloroplast genomeswith those of other species in theMalvaceae revealed breakpoints in the accD locus,which is involved in fatty acid synthesis,in C.capsularis and C.olitorius.This finding suggests that genes from the chloroplast genomemight have been transferred to the nuclear genome in some Corchorus species.This hypothesis was supported by synteny analysis of the accD region among the nuclear,chloroplast,and mitochondrial genomes.To our knowledge,this is the first report of the assembled chloroplast genome sequences of C.capsularis and C.olitorius.C.capsularis and C.olitorius are closely related to Gossypium species and there are abundant microstructure variations between these two genera.These results will expand our understanding of the systematics of species in the Malvaceae.

Tris(trimethylsilyl) borate as an electrolyte additive for high-voltage lithium-ion batteries using LiNi_(1/3)Mn_(1/3)Co_(1/3)O_2 cathode

The influence of tris(trimethylsilyl) borate (TMSB) as an electrolyte additive on lithium ion cells have been studied using Li/LiCo1/3Ni1/3Mn1/3O2 cells at a higher voltage, 4.7 V versus Li/Li+. 1 wt% TMSB can dramatically reduce the capacity fading that occurs during cycling at room temperature (RT) and elevated temperature (60 degrees C). After 150 cycles at 1 C rate (1 C= 278 mAh/g), the capacity retention of Li/LiCo1/3Ni1/3Mn1/3O2 is up to near 72% in the electrolyte with TMSB added, while it is only about 35% in the baseline electrolyte. The electrochemical behaviors, the surface chemistry and structure of Li/LiCo1/3Ni1/3Mn1/3O2 cathode are characterized with charge/discharge test, linear sweep voltammetry (LSV), X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), thermal gravimetric analyses (TGA), scanning electron microscope (SEM) and transmission electron microscopy (TEM). These analysis results reveal that the addition of TMSB is able to protectively modify the electrode CEI film in a manner that suppresses electrolyte decomposition and degradation of electrode surface structure, even though at both a higher voltage of 4.7 V and an elevated temperature of 60 degrees C. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

Pt nanodendrites with a PtIr alloy surface structure exhibit excellent stability toward acidic hydrogen evolution reaction

The development of effective and stable electrocatalysts for the hydrogen evolution reaction(HER)in acidic electrolytes is a significant challenge.In this work,homogeneous Pt nanodendrites(Pt NDs)with a PtIr shell were successfully synthesized by a two-step wet chemical method.This open three-dimensional(3D)dendritic structure exhibited exceptional electrocatalytic characteristics,exposing as many active sites as feasible.Furthermore,by alloying Ir with Pt on the surface,catalytic activity was greatly enhanced while ensuring extremely high stability.Iridium surface-enriched platinum nanodendritic catalysts(Pt@PtIr NDs)outperformed the control samples and the commercial catalysts.In acidic HER test,Pt@PtIr NDs had a lower overpotential(22 mV)than Pt NDs(26 mV)and commercial Pt/C(31 mV)at 10 mA/cm^(2),and the activity of Pt@PtIr NDs remained consistent even after undergoing a continuous durability test for at least 168 h,which was much superior to the performance of commercial Pt/C(10 h)under identical test conditions.This study revealed that the application of 3D Pt dendritic metal alloys may offer a chance for the development of enhanced electrocatalysts in acidic HER.

分割氢键有机框架的孔道空间提升光催化CO_(2)还原效率

氢键有机框架材料(HOFs)在催化领域具有巨大的潜力,但其孔道空间在去除溶剂后易塌陷,限制了其在光催化能源转换和存储方面的应用.本研究采用孔道分割策略成功设计并合成了一种稳定孔道结构、高效光催化CO_(2)还原活性的HOF催化剂.H4TBAPy分子通过与HOF孔道中大量的CH…π相互作用锚定自身,并将HOF的大孔道分隔成多个小空间,显著增加了HOF框架的稳定性.同时,富电子属性的H4TBAPy分子提升了HOF体系中电子的传输速率,从而提高了催化活性.这项研究为设计稳定、高性能的HOFs光催化剂提供了新策略.

X-ray excited Mn^(2+)-doped persistent luminescence materials with biological window emission for in vivo bioimaging

In recent years,persistent luminescence materials(PLMs)excited by X-rays and emitting in biological windows have received extensive attention in the field of high-sensitivity bioimaging.Transition metal Mn^(2+)is an ideal emission center,but few studies focus on Mn^(2+)-doped PLMs with X-ray excitation and biological window emission.Here,we report a Mn^(2+)-doped PLM,LiYGeO_(4):Mn^(2+)(LYGM),with excellent biological window persistent luminescence emission.After excitation by UV,LYGM produces a durable biological window of persistent luminescence emission at 660 nm for up to 20 h.More importantly.LYGM can be repeatedly excited by X-rays,resulting in long-term biological window persistent luminescence emission.In addition,we obtain LYGM around 200 nm in diameter by ball milling and centrifugation and improve its biocompatibility by surface modification to apply it to in vivo imaging in mice.After LYGM are injected into mice through the tail vein,in situ excitation of X-rays can be achieved.After the persistent luminescence decays,LYGM can be re-excited for repeated imaging.Therefore,LYGM shows potential prospects for in vivo deep tissue and long-term bioimaging.

Highly crystallization-induced emissive luminophores with mechanoluminescent features for two-photon harvesting fluorescence imaging and latent fingerprint identification

Fluorescence imaging can be employed in fields of medical treatment,astronomical exploration,and national defense security.Traditional fluorescence imaging often takes the single-photon techniques,which is vulnerable to background interference and photobleaching.Remedially,two-photon fluorescence imaging can achieve much higher-resolution fluorescence imaging for reducing scattering and deeper depth.Hence,by assembling the tetraphenylethylene backbones with nontoxic and non-noble K^(+)ions,compound 1([(Hdma)K(H_(2)ettc)]_(n),H_(4)ettc=4',4''',4''''',4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis(([1,1'-biphenyl]-4-carboxylic acid)))with the crystallization-induced emissions exhibited charming fluorescence imaging under two-photon excitation microscopy(TPEM).Besides,luminescent powders based on compound 1 can achieve high-resolution fingerprint recognition,providing secure access control and identification for a novel authentication method.Compared with the commercial fluorescent dyes coumarin-6,the as-synthesized compound 1 showed great solvent stability,indicating its durability against harsh environment.Moreover,compound 1 shows mechanoluminescent properties for the perturbation of weak supramolecular interactions within ordered arrangements of the H_(2)ettc^(2−)ligands.This novel compound has provided an important insight to the development of twophoton fluorescence imaging and advanced external-stimuli responsive materials.

Free amino group-directed C(sp^(2))-H arylation ofα-amino-β-aryl esters by palladium catalysis

Native amino-directed palladium-catalyzed C(sp^(3))-H activation/functionalization has been developed for modification ofα-amino acids and peptides.Herein a palladium(Ⅱ)-catalyzed C(sp^(2))-H arylation ofα-amino-β-aryl esters has been disclosed,using the native amino as the directing group.A variety of chiralα-amino-β-aryl esters can be functionalized to give the corresponding ortho-substituted mono-and di-arylated products.

High-resolution remote thermometry based on Bi^(3+)-doped 0D zinc halide hybrids

Developing highly sensitive optical thermometers is of great significance due to their capability to enable remote and non-contact temperature measurements, rendering them highly applicable in diverse and harsh environments. Herein we report a temperature-dependent phosphor of 0D metal halide hybrid by incorporating Bi^(3+)into the(MePPh_(3))_(2)ZnCl_(4) matrix. Through Bi^(3+)doping,the initially non-luminescent(MePPh_(3))_(2) ZnCl_(4) matrix exhibits a deep-blue emission centered at 453 nm, with a photoluminescence quantum yield(PLQY) of 5.71% and a Stokes shift of 75 nm at room temperature. Experimental characterization demonstrates that exciton-like luminescence of Bi^(3+)is mainly responsible for the blue emission. Single crystals of Bi^(3+)-doped(MePPh_(3))_(2)ZnCl_(4) show an unusual correlation between photoluminescence(PL) lifetime and temperature. Particularly, the dependence of luminescence lifetime on temperature is most remarkable in the temperature range of 80 to 100 K with an exceptional sensitivity up to 0.09 K^(-1), representing one of the best levels for thermometry based on PL decay lifetime. Our work not only provides a viable strategy for designing a novel, environmentally friendly, and stable blue emitter, but also paves the way for precise thermometric application at low temperature.

Plasmon-enhanced photocatalytic oxidative coupling of amines in the air using a delicate Ag nanowire@NH_(2)-UiO-66 core-shell nanostructures

MOF-based core-shell structures with high surface area, abundant active sites, and broad absorption bands are viable alternatives to traditional single-component photocatalysts. In this report, we describe the design and construction of delicate Ag nanowires@NH_(2)-UiO-66 with a core-shell structure for use as photocatalysts in imine synthesis under light. The optimized composites exhibited 80% imine production, which was higher than both MOF and Ag NWs. The significant improvement in photocatalytic activity under light may be attributed to the plasmonic effect of silver nanowires and their core-shell structure, which promotes the separation of electron-hole pairs. Moreover, the photocatalytic activity of the core-shell nanostructure may provide valuable insight into the design and construction of MOF-based composite photocatalysts for oxidative coupling of amines.

X-ray-activated Bi^(3+)/Pr^(3+)co-doped LiYGeO_4 phosphor with UV and NIR dual-emissive persistent luminescence

X-ray-activated luminescence materials have broad application prospects in photodynamic therapy of deep tissue.Among them,X-ray-activated persistent luminescence materials(PLMs)exhibiting multiple emission peaks have drawn extensive attention for the ir capacity to achieve a combination of bioimaging and therapeutic functions.Here,we developed a novel PLM,LiYGeO_4:Bi^(3+),Pr^(3+),that simultaneously exhibits UV and NIR dual persistent luminescence(PersL)emissions after irradiation by X-ray.The material can be re peatedly excited by X-ray and emits similar lumine scence intensity every time,which shows good PersL stability.In addition,LiYGeO_4:Bi^(3+),Pr^(3+)exhibits photostimulated PersL properties by stimulation with a red light-emitting diode(LED)or NIR laser after long-term decay.This work provides a new choice of X-ray-excited PLMs with UV and NIR dual emission and the novel phosphor shows promise as a potential candidate for the integration of treatment and diagnosis of deep tumors.

"刚柔并济"构筑可"劈裂"光的高稳定性晶体材料

There is a pressing demand for the development of novel birefringent crystals tailored for compact optical components,especially for crystals exhibiting large birefringence across a range of temperatures.This has commonly been achieved by introducing various deformable groups with high polarizability anisotropy.In this study,we combined both rigid and deformable groups to synthesise a new birefringent crystal,Al_(2)Te_(2)MoO_(10),which demonstrates an exceptional birefringence value of 0.29@550 nm at room temperature.Not only is this higher birefringence than that of commercial crystals,but Al_(2)Te_(2)MoO_(10)exhibits excellent birefringence stability over a wide temperature range,from 123 to 503 K.In addition,the first-principles theory calculations and structural analyses suggest that although the rigid AlO_(6)groups do not make much contribution to the prominent birefringence,they nonetheless played a role in maintaining the structural anisotropy at elevated temperatures.Based on these findings,this paper proposes a novel structural design strategy to complement conventional approaches for developing optimal birefringent crystals under various environmental conditions.

Efficient Spin-Flip between Charge-Transfer States for High-Performance Electroluminescence, without an Intermediate Locally Excited State

Thermally activated delayed fluorescence(TADF)materials with both high photoluminescence quantum yield(PLQY)and fast reverse intersystem crossing(RISC)are strongly desired to realize efficient and stable organic light-emitting diodes(OLEDs).Control of excited-state dynamics via molecular design plays a central role in optimizing the PLQY and RISC rate of TADF materials but remains challenging.Here,3 TADF emitters possessing similar molecular structures,similar high PLQYs(89.5%to 96.3%),and approximate energy levels of the lowest excited singlet states(S_(1)),but significantly different spin-flipping RISC rates(0.03×10^(6) s^(−1) vs.2.26×10^(6) s^(−1))and exciton lifetime(297.1 to 332.8μs vs.6.0μs)were systematically synthesized to deeply investigate the feasibility of spin-flip between charge-transfer excited states(^(3)CT–^(1)CT)transition.

Ultralong Organic Phosphorescence of Triazatruxene Derivatives for Dynamic Data Encryption and Anti-counterfeiting

Comprehensive Summary,Organic luminogens with persistent room temperature phosphorescence(RTP)have drawn tremendous attentions due to their promising potentials in optoelectronic devices,information storage,biological imaging,and anti-counterfeiting.In this work,six triazatruxene-based lumiogens with different peripheral substituents and configurations are synthesized and systematically studied.The results show that their fluorescence quantum yields in solid states range from 15.73%to 37.58%.Dispersing the luminogens as guest into the host(PPh_(3))could turn on the persistent RTP,where PPh_(3)acts as not only a rigid matrix to suppress the non-radiative transitions of the guest,but also provides energy transfer channels to the guest.The maximum phosphorescence efficiency and the longest lifetime could reach 29.35%and 0.99 s in co-crystal films of 6-TAT-CN/PPh_(3)and 5-TAT-H/PPh_(3),respectively.Moreover,these host-guest co-crystalline films exhibit great potentials in advanced dynamic data encryption and anti-counterfeiting.This work deepens the insight for low cost,halogen-free,and facile fabrication of all-organic persistent RTP materials.

Nd:YAG linearly polarized laser based on polarization eigenmodes

In this paper,the frequency difference of the eigen polarization modes of the Nd:YAG crystal laser at different polarization ratios is experimentally studied,and to the best of our knowledge,the correlation between the frequency difference of the eigenmodes and the output polarization degree is reported for the first time.Combined with the analysis of the polarization beam profile,it is proved that the polarized laser produced by the isotropic crystal is due to the frequency locking of the eigen polarization modes.The weak birefringence in the crystal causes the round-trip phase difference of the orthogonal polarization modes,which leads to the frequency difference between the polarization modes.By the adjustment of the cavity mirror,the anisotropic loss will interact with the round-trip phase difference.The eigen polarization modes can reach frequency degeneration,and then be coherently combined to produce linearly polarized laser output.This work provides a useful reference for understanding the physical mechanism of polarized lasers realized by isotropic crystals.

Boosting Electrocatalytic CO_(2)Reduction with Conjugated Bimetallic Co/Zn Polyphthalocyanine Frameworks

Development of high-efficiency electrode materials for the electrochemical CO_(2)reduction reaction(CO_(2)RR)with high current density and selectivity compatible with industry is an important but significant challenge.Herein,we describe a facile strategy to enhance the selectivity and current density by regulating the local electron density of the cobalt site in a series of stable,conjugated,bimetallic Co/Zn polyphthalocyanine frameworks Co_(x)Zn_(y)PPc with an AB stacking model under alkaline aqueous conditions.When adjusting the ratio of Co and Zn to 3:1,the optimal Co3Zn1PPc exhibits an industry-compatible CO partial current density of 212 mA cm^(−2)at−0.9 V versus reversible hydrogen electrode in a flow cell,which is 1.7 and 9.1 times that of the single metal polyphthalocyanine CoPPc and ZnPPc,respectively.Co_(3)Zn_(1)PPc shows a high CO Faraday efficiency of more than 90%in a wide operating potential window of−0.3 to−0.9 V.In-depth experimental and theoretical analysis revealed that introduction of electron-rich Zn atoms modified the electron density of the active Co center,placing Co in the electronrich region and weakening the bonding strength with the reaction intermediate,thereby improving the CO_(2)RR performance.These results clarify the interaction mechanism of dual metal sites at the atomic level and provide a new avenue for the design of electrocatalysts with potential in industrial applications.

The visible light-triggered nonvolatile memory performances in melamine-decorated <110>-oriented lead halide perovskites: A photo-responsive structural evolution insight

The exploration of novel photo/thermal-responsive nonvolatile memorizers will be beneficial for energysaving memories.Herein,new<110>-oriented perovskites using single template melamine,i.e.,[(MLAI-H_(2))(PbX_(4))]_n(X=Br (α-1),Cl (α-2),MLAI=melamine) have been prepared and their structures upon irradiation of visible light have been investigated.They have been fabricated as nonvolatile memory devices with structures of ITO/[(MLAI-H_(2))(PbX_(4))]_n/PMMA/Ag (device-1:X=Br,device-2:X=Cl),which can exhibit unique visible light-triggered binary nonvolatile memory performances.Interestingly,the silent or working status can be monitored by visible chromisms.Furthermore,the light-triggered binary resistive switching mechanisms of these ITO/[(MLAI-H_(2))(PbX_(4))]_n/PMMA/Ag memory devices have been clarified in terms of EPR,fluorescence,and single-crystal structural analysis.The presence of light-activated traps in<110>-oriented[(MLAI-H_(2))(PbX_(4))]_n perovskites are dominated in the appearance of light-triggered resistive switching behaviors,based on which the inverted internal electrical fields can be established.According to the structural analysis,the more distorted PbX_6octahedra,higher corrugated<110>-oriented perovskite sheets,and more condensed organic-inorganic packing in Br-containing perovskite are beneficial for the stabilization of light-activated traps,which lead to the better resistive switching behavior of device-1.This work can pave a new avenue for the establishment of novel energy-saving nonvolatile memorizers used in aerospace or military industries.

The effects of local environment towards yield and selectivity on photocatalytic CO_(2)reduction catalyzed by metal-organic framework

The CO_(2)photoconversion is sensitive to the local reaction environment,of which activity and selectivity can be regulated by the change of reaction systems.This paper focuses on investigating the photocatalytic CO_(2)reduction behaviors of MOFs with the involvement of water under different reaction modes,including gas-solid and liquid-solid systems.The CO_(2)photoreduction in a liquid-solid system shows high performance in generating HCOOH with the selectivity of 100%.In contrast,the gas-solid system referring to the synergistic interaction of MOFs and H_(2)O vapor benefits to the formation of gas-phase products,such as CO and CH_(4).The possible mechanisms of photocatalytic CO_(2)reaction in two modes were investigated by in-situ Fourier-transform infrared spectroscopy,which indicates that the distinction in reaction consequence may result from the difference in CO_(2)chemisorbed modes and the proton provision.The choice of reaction system plays an important role in the achievement of high efficiency and selectivity for photocatalytic CO,reduction,whichis of great practical value in real-world applications.

Post-modification of metal-organic framework for improved CO_(2) photoreduction efficiency

Utilizing metal-organic frameworks(MOFs) to design photocatalysts for CO_(2) reduction catalysts is an excellent idea but currently restricted by the relatively low activity. Enhancing CO_(2) affinity and tuning the oxidation state of metal clusters in MOFs might be a solution to improve the catalytic performance.Herein, the Cl-bridge atoms in the metal clusters of a cobalt MOF were easily exchanged with OH-,which simultaneously oxidized a portion of Co(Ⅱ) to Co(Ⅲ) and resulted in a much enhanced photocatalytic activity for CO_(2) reduction. In contrast, the original framework does not exhibit such superior activity. Comprehensive characterizations on their physicochemical properties revealed that the introduction of hydroxyl group not only greatly increases the CO_(2) affinity but also alters the oxidation state of metal clusters, resulting in significantly improved photocatalytic activities for CO_(2) reduction. This work provides important insight into the design of efficient photocatalysts.

Maximizing the linear and nonlinear optical responses of alkaline tricyanomelaminate

High-performance bi-functional materials are in urgent demand for the next-generation integrated optical devices.In this work,we successfully synthesized the first tricyanomelaminate with bi-functional optical responses,namely Cs_(3)C_(6)N_(9)•H_(2)O(I),from its analogue Na_(3)C_(6)N_(9)•3H_(2)O by a facile ion exchange method.In contrast to Na_(3)C_(6)N_(9)•3H_(2)O,I realizes an optimal arrangement of𝜋π-conjugated(C_(6)N_(9))3−anion groups in its crystal structure.As a result,the second-order nonlinear optical(NLO)response is greatly enhanced from nearly zero of Na_(3)C_(6)N_(9)•3H_(2)O to∼9.8×KH_(2)PO_(4)of I.Furthermore,I exhibits a giant linear optical anisotropic response(i.e.birefringence)of 0.52 at the wavelength of 550 nm.Both responses are almost the largest among the inorganic compounds ofπ-conjugated rings,which indicates that I has great potential as a bi-functional optical crystal.Structural and theoretical analyses reveal the microscopic origin of excellent optical properties.This work would attract a lot of interest to the persistently neglected potential of tricyanomelaminates as linear optical and NLO crystals.