Miniaturized electrochemical sensors and their point-of-care applications

Most of the current analytical methods depend largely on laboratory-based analytical techniques that require expensive and bullky equipment,potentially incur costly testing,and involve lengthy detection processes.With increasing requirements for point-of-care testing(POCT),more attention has been paid to miniaturized analytical devices.Miniaturized electrochemical(MEC)sensors,including different material-based MEC sensors(such as DNA-,paper-,and screen electrode-based),have been in strong demand in analytical science due to their easy operation,portability,high sensitivity,as well as their short analysis time.They have been applied for the detection of trace amounts of target through measuring changes in electrochemical signal,such as current,voltage,potential,or impedance,due to the oxidation/reduction of chemical/biological molecules with the help of electrodes and electrochemical units.MEC sensors present great potential for the detection of targets including small organic molecules,metal ions,and biomolecules.In recent years,MEC sensors have been broadly applied to POCT in various fields,including health care,food safety,and environmental monitoring,owing to the excellent advantages of electrochemical(EC)technologies.This review summarized the state-of-the-art advancements on various types of MEC sensors and their applications in POCT.Furthermore,the future perspectives,opportunities,and challenges in this field are also discussed.     

Machine Learning towards Screening Solid-state Lithium Ion Conductors

Machine learning is an emerging method to discover new materials with specific characteristics.An unsupervised machine learning research is highlighted to discover new potential lithium ionic conductors by screening and clustering lithium compounds,providing inspirations for the development of solid-state electrolytes and practical batteries.     

等浓度的氯化铵和硫酸铵溶液哪个pH高

有中学化学参考资料题:0.10 mol/L的NH4Cl和(NH4)2SO4溶液哪个pH值高?这似乎是个中学生可做的简单题目,仔细考虑不是如此.如果简单地认为盐酸和硫酸都是强酸,而硫酸是二元酸,硫酸铵溶液中铵盐浓度为0.20 mol/L,那么NH4Cl溶液pH高,那是不妥的.硫酸是二元酸,第一个氢离子能完全电离,第二个氢离子部分电离,如此考虑情况怎么样呢?是不是答案发生变化?这要通过计算来说明.     

Surface defect-rich ceria quantum dots anchored on sulfur-doped carbon nitride nanotubes with enhanced charge separation for solar hydrogen production

Designing defect-engineered semiconductor heterojunctions can effectively promote the charge carrier separation.Herein,novel ceria(CeO2) quantum dots(QDs) decorated sulfur-doped carbon nitride nanotubes(SCN NTs) were synthesized via a thermal polycondensation coupled in situ depositionprecipitation method without use of template or surfactant.The structure and morphology studies indicate that ultrafine CeO2 QDs are well distributed inside and outside of SCN NTs offering highly dispersed active sites and a large contact interface between two components.This leads to the promoted formation of rich Ce³⁺ ion and oxygen vacancies as confirmed by XPS.The photocatalytic performance can be facilely modulated by the content of CeO2 QDs introduced in SCN matrix while bare CeO2 does not show activity of hydrogen production.The optimal catalyst with 10% of CeO2 loading yields a hydrogen evolution rate of 2923.8 μmol h-1 g-1 under visible light,remarkably higher than that of bare SCN and their physical mixtures.Further studies reveal that the abundant surface defects and the created 0 D/1 D junctions play a critical role in improving the separation and transfer of charge carriers,leading to superior solar hydrogen production and good stability.     

Superfast and solvent-free core-shell assembly of sulfur/carbon active particles by hail-inspired nanostorm technology for high-energy-density Li-S batteries

The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^-2 delivers a stable area capacity of 6.6 mAh cm^-2 over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^-2 over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.     

Unraveling the stabilization mechanism of solid electrolyte interface on ZnSe by rGO in sodium ion battery

Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.     

CXN天然沸石的研究2: 吸附性质

采用N~2,NH~3,CO~2,乙烯,丙烯,水,甲醇,乙醇,丙醇等作为吸附剂,研究了由我国CXN天然沸石改性制得的H-STI和Na-STI沸石的吸附性质,H-STI和Na-STI沸石的BET表面积及微孔孔体积约为420m^2/g和0.20m^3/g。根据NH~3和CO~2在H-STI沸石上的吸附等温线计算得到它们的吸附热分别为44.8和26.5kJ/mol。乙烯,丙烯,甲醇,乙醇,丙醇等在Na-STI沸石上的吸附等温线表明该沸石对有机分子的吸附具有链长选择性。在低分压下水相对于甲醇的吸附量表明沸石具有一定的疏水性质。     

常温常湿条件下Au/MeO~x催化剂上CO氧化性能

利用共沉淀法制备了Au/MeO~x催化剂(Me=Al,Co,Cr,Cu,Fe,Mn,Ni,Zn)。在常温常湿条件下,考察了不同氧化物负载的金基催化剂的CO氧化性能。结果表明,氧化物种类对催化剂的活性和稳定性均有较大的影响。Cu,Mn,Cr等氧化物负载的金基催化剂的活性较差,而Zn,Fe,Co,Ni,Al等金属氧化物负载的金基催化剂可将CO完全氧化,又具有一定的稳定性,在相同反应条件下,CO完全转化时的稳定性顺序为Au/ZnO>Au/α-Fe~2O~3>Au/Co~3O~4>Au/γ-Al~2O~3≈Au/NiO。还发现水对Au/MnO~x催化剂的活性和稳定性有负作用,而对180℃焙烧制备的Au/ZnO-180催化剂的活性和稳定性均有明显的湿度增强作用。     

Enhanced efficiency and stability in Sn-based perovskite solar cells with secondary crystallization growth

The conversion efficiencies reported for Tin(Sn)halide-based perovskite solar cells(PSCs)fall a large gap behind those of lead halide-based PSCs,mainly because of poor film quality of the former.Here we report an efficient strategy based on a simple secondary crystallization growth(SCG)technique to improve film quality for tin halide-based PSCs by applying a series of functional amine chlorides on the perovskite surface.They were discovered to enhance the film crystallinity and suppress the oxidation of Sn²⁺remarkably,hence reduce trap state density and non-irradiative recombination in the absorber films.Furthermore,the SCG film holds the band levels matching better with carrier transport layers and herein favoring charge extraction at the device interfaces.Consequently,a champion device efficiency of 8.07% was achieved alo ng with significant enhancements in VOC and JSC,in contrast to 5.35% of the control device value.Moreover,the SCG film-based devices also exhibit superior stability comparing with the control one.This work explicitly paves a novel and general strategy for developing high performance lead-free PSCs.     

Boost oxygen reduction reaction performance by tuning the active sites in Fe-N-P-C catalysts

Cost-effective atomically dispersed Fe-N-P-C complex catalysts are promising to catalyze the oxygen reduction reaction(ORR)and replace Pt catalysts in fuel cells and metal-air batteries.However,it remains a challenge to increase the number of atomically dispersed active sites on these catalysts.Here we report a highly efficient impregnation-pyrolysis method to prepare effective ORR electrocatalysts with large amount of atomically dispersed Fe active sites from biomass.Two types of active catalyst centers were identified,namely atomically dispersed Fe sites and Fe_xP particles.The ORR rate of the atomically dispersed Fe sites is three orders of magnitude higher than it of Fe_xP particles.A linear correlation between the amount of the atomically dispersed Fe and the ORR activity was obtained,revealing the major contribution of the atomically dispersed Fe to the ORR activity.The number of atomically dispersed Fe increases as the Fe loading increased and reaching the maximum at 1.86 wt%Fe,resulting in the maximum ORR rate.Optimized Fe-N-P-C complex catalyst was used as the cathode catalyst in a homemade Zn-air battery and good performance of an energy density of 771 Wh kgZn^-1,a power density of 92.9 m W cm^-2 at 137 m A cm^-2 and an excellent durability were exhibited.     

Synthesis of Eu3+-doped core and core/shell nanoparticles and direct spectroscopic identification of dopant sites at the surface and in the interior of the particles

A variety of redispersible Eu(3+)-doped LaPO(4) nanoparticles have been prepared in a high-boiling coordinating solvent mixture, and the Eu(3+) lattice sites of these materials have been investigated by luminescence line-narrowing measurements. In this spectroscopic method, Eu(3+) ions occupying different lattice sites are selectively excited with a tunable narrow-bandwidth laser system and distinguished by their luminescence spectra ("site-selective spectroscopy"). Depending on the concentration of the dopant, up to three different lattice sites could be identified in the interior of the LaPO(4) nanoparticles. These sites correspond to those known from bulk LaPO(4). In addition, a variety of surface sites is observed, which could be converted completely into bulk sites by overgrowing the nanoparticles with a shell of pure LaPO(4). The surface sites are identical to those obtained by reacting Eu(3+) with the surface of pure LaPO(4) nanoparticles. The spectroscopic properties of Eu(3+)-doped LaPO(4) nanoparticles differ from those of pure EuPO(4) nanoparticles, which were also investigated. Remarkably, the core/shell synthesis investigated in this paper allows one to prepare doped nanoparticles that contain no other dopant sites than those known from the corresponding bulk material.     

沉淀转化法制备多孔片状纳米LaF3

采用实验中所合成的LaPO4纳米棒为前驱体,通过沉淀的转化作用,大面积地制备了单分散的片状纳米LaF3。采用扫描电镜(SEM)、透射电镜(TEM)、X射线衍射仪(XRD)、BET(Brunauer-Emmett-Teller)测试对片状纳米LaF3的形貌、结构、相组成及表面性质进行了分析。片状纳米LaF3底边长约为40 nm,片的厚度约为35 nm,大小均一,具有多孔结构。通过改变反应溶剂,可以控制LaF3粒子的成核、生长和团聚,从而有效地调控多孔片状纳米LaF3的颗粒尺寸和分散性。对多孔片状纳米LaF3的生长机制进行了研究,结果表明LaPO4和LaF3的溶度积常数差导致了片状纳米LaF3的生成;体系中自身存在的Ostwald ripening作用使片状纳米LaF3出现了多孔结构。     

液相浸渗法制备Y-TZP/LaPO4可加工复相陶瓷

通过往ZrO2多孔陶瓷浸渗LaPO4液态先驱液制备了具有可加工性的Y－TZP／LaPO4复相陶瓷。加入30％（体积分数）石墨可以得到具有35％（体积分数）开孔气孔率的ZrO2预烧结陶瓷体。采用不同浸渗和热分解周期可以得到不同LaPO4含量的Y－TZP／LaPO4复相陶瓷。研究了该材料的可加工性和力学性能。结果表明，含有3.5%-7.5%(体积分数）LaPO4的Y－TZP／LaPO4复相陶瓷具有良好的可加工性，同时保持优良的力学性能。     

Eu~(3+)-doped LaPO_4 and LaAlO_3 nanosystems and their luminescence properties

Eu3+ ion-doped LaPO4 nanowires or nanorods have been successfully synthesized by a simple hydrothermal method.The influence of varying the hydrothermal and subsequent sintering conditions on the morphology and structure of the LaPO4 host has been investigated by scanning electron microscopy(SEM) and X-ray diffraction(XRD).For comparison,the Eu3+ ions were also doped into monoclinic monazite LaPO4 nanoparticles and perovskite LaAlO3 nanoparticles.The relative intensities of the emission lines of the LaPO4:Eu...     

低成本LaPO4-LnPO4核壳结构荧光颗粒的合成与表征

LnPO4( LnPO4=LaPO4:Ce,Tb)是被广泛应用的绿色荧光材料,由于所用的主要原材料之一Tb4O7的价格较为昂贵,导致其生产成本居高不下.如能有效合理地降低稀土磷酸盐绿色荧光粉的生产成本,则可望为照明工业带来显著的效益.报道了一种新型的核壳结构材料LaPO4-LnPO4,该材料以较为廉价的LaPO4作为内部核层,三聚磷酸盐水解缓慢释放的磷酸根与稀土离子通过均相沉淀异相成核的方法在LaPO4表面结合形成LnPO4壳层.所得核壳结构颗粒的荧光发射光谱与纯LnPO4完全一致.在还原性气氛中灼烧后,其发光强度可与市售LnPO4商业产品相当.本方法可将稀土磷酸盐绿色荧光粉的合成成本降低45％左右,而且操作简单,易于进行大规模工业化生产推广,对发光照明行业具有潜在的重要应用价值.     

共沉淀法合成稀土正磷酸盐(La,Gd)PO4:RE3+(RE=Eu,Tb)及其真空紫外光谱特性

采用共沉淀法制备了稀土正磷酸盐荧光粉(La,Gd)PO4:RE3+(RE=Eu,Tb).红外光谱分析发现GdPO4的红外光谱吸收峰与LaPO4一致,只是峰位向高波数方向移动.(La,Gd)PO4:RE3+的真空紫外光谱特性研究表明,Gd3+在能量传递过程中起中间体作用.XPS研究揭示,LaPO4的价带由O2-的2p能级构成,而GdPO4的价带则是由O2-的2p能级和Gd3+的4f能级共同构成.     

Epitaxial synthesis of uniform cerium phosphate one-dimensional nanocable heterostructures with improved luminescence

Uniform CePO(4)@LaPO(4) and CePO(4):Tb(3+)@LaPO(4) one-dimensional single-crystalline nanocable heterostructures with highly enhanced photoluminescent emission have been synthesized via a mild and simple hydrothermal approach. The resulting one-dimensional single-crystalline nanocable heterostructures have smooth and uniform LaPO(4) sheaths, which is of great significance in effectively eliminating surface trap-states and suppressing the energy quenching in energy-transfer processes. The photoluminescence results for these one-dimensional nanocable heterostructures illustrate that the uniform LaPO(4) sheaths remarkably increase the luminescent efficiency.     

季铵盐修饰磷钼酸铵纳米微粒的制备、结构表征及摩擦学性能

在醇 -水体系中采用同阴离子共沉淀法制备了季铵盐修饰的 (NH4 ) 3PMo12 O4 0 纳米微粒 ,采用TEM ,XRD ,FTIR ,TGA&DSC等多种分析手段表征了这种纳米微粒的形貌和结构 ,在四球试验机上考察了它们的摩擦学性能。结果表明所合成的杂多化合物具有Keggin骨架结构 ,微粒粒径约 2 0nm ,在有机溶剂中可良好分散 ,作为一类新型润滑油添加剂 ,具有良好的抗磨性能。     

基于LaPO_4∶Ce,Tb-Au发光共振能量转移测定细胞色素C

以膦酰基羧酸共聚物为修饰剂,采用水热法制备了LaPO_4∶Ce,Tb发光纳米粒子,该粒子具有良好的水溶性和生物相容性。对合成的纳米粒子进行了发光光谱、X-射线衍射、透射电子显微镜和红外光谱表征。以制备的纳米粒子为能量供体,纳米金为能量受体,细胞色素C(Cyt C)为桥,构建了LaPO_4∶Ce,Tb-Au发光共振能量转移(LRET)体系,据此建立了测定Cyt C的新方法。实验结果表明,当Cyt C的浓度在0.333~21.0μg·mL~(-1)范围时,LRET体系发光猝灭程度与Cyt C浓度呈良好线性关系,检出限(S/N=3)为0.2μg·mL~(-1),相对标准偏差(RSD)为0.46%(c=10.0μg·mL~(-1),n=11)。该方法用于实际样品的测定,回收率范围为100%~101%。     

A simple mixed-solvothermal route for LaPO4 nanorods: synthesis, characterization, affecting factors and PL properties of LaPO4:Ce3+

In this paper, LaPO(4) nanorods have been successfully synthesized via a simple water-ethyleneglycol (H(2)O-EG) mixed-solvothermal route, employing lanthanum nitrate (La(NO(3))(3)·xH(2)O) as a La(3+) ion source and monobasic sodium phosphate (NaH(2)PO(4)·2H(2)O) as a PO(4)(3-) ion source. The as-obtained products were characterized by means of X-ray powder diffraction (XRD), energy dispersive spectrometry (EDS), (high resolution) transmission electron microscopy (HR/TEM), selected area electron diffraction (SAED) and field emission scanning electron microscopy (FESEM). Some factors influencing the formation of LaPO(4) nanorods, including the reaction temperature, the volume ratio of water/EG and the original amount of H(2)PO(4)(-) ions, were investigated. Experiments showed that the volume ratio of water/EG and the original amount of H(2)PO(4)(-) ions could markedly affect the morphology of the final product.