Interfacial built-in electric field and crosslinking pathways enabling WS_(2)/Ti_(3)C_(2)T_(x) heterojunction with robust sodium storage at low temperature

Developing efficient energy storage for sodium-ion batteries(SIBs)by creating high-performance heterojunctions and understanding their interfacial interaction at the atomic/molecular level holds promise but is also challenging.Besides,sluggish reaction kinetics at low temperatures restrict the operation of SIBs in cold climates.Herein,cross-linking nanoarchitectonics of WS_(2)/Ti_(3)C_(2)T_(x) heterojunction,featuring built-in electric field(BIEF),have been developed,employing as a model to reveal the positive effect of heterojunction design and BIEF for modifying the reaction kinetics and electrochemical activity.Particularly,the theoretical analysis manifests the discrepancy in work functions leads to the electronic flow from the electron-rich Ti_(3)C_(2)T_(x) to layered WS_(2),spontaneously forming the BIEF and“ion reservoir”at the heterogeneous interface.Besides,the generation of cross-linking pathways further promotes the transportation of electrons/ions,which guarantees rapid diffusion kinetics and excellent structure coupling.Consequently,superior sodium storage performance is obtained for the WS_(2)/Ti_(3)C_(2)T_(x) heterojunction,with only 0.2%decay per cycle at 5.0 A g^(-1)(25℃)up to 1000 cycles and a high capacity of 293.5 mA h g^(-1)(0.1A g^(-1)after 100 cycles)even at-20℃.Importantly,the spontaneously formed BIEF,accompanied by“ion reservoir”,in heterojunction provides deep understandings of the correlation between structure fabricated and performance obtained.

Synthesis of Mesoporous Chromium Aluminophosphate (CrAlPO) via Solid State Reaction at Low Temperature

Mesoporous chromium aluminophosphate （CrAIPO） was successfully synthesized via solid state reaction （SSR） route at low temperature in the presence of a cationic surfactant cetyltrimethyl ammonium bromide （CTAB） and inorganic sources such as A1C13 · 6H20, CrCI3 · 6H20 and NaH2PO4 · 2H20. Characterizations by means of powder X-ray diffraction （XRD）, N2 adsorption- desorption, high resolution transmission electron microscopy （HR-TEM）, scanning electron micrography （SEM）, energy dispersion spectroscopy （EDS）, thermo-gravimetry （TG）, Fourier transform infrared spectroscopy （FT-IR）, and ultraviolet visible light spectroscopy （UV-Vis） were carried out to understand both the pore characteristics and electron transition route of these obtained materials. The experimental results show that the meso-CrA1PO materials with various Cr/A1 molar ratios possess a mesostructure and a specific surface area of 193 to 310 m2/g corresponding to an average pore size of 5.5 to 2.2 rim, respectively. The maxium content of Cr in meso-CrA1PO materials synthesized via SSR route can achieve 16.7wt%, being significantly higher than that of the meso-CrA1PO prepared via a conventional sol-gel route. Meanwhile, the formation mechanism of the meso-CrA1PO was also proposed.

Doping effect of cations(Zr^(4+),Al^(3+),and Si^(4+)) on MnO_x/CeO_2 nano-rod catalyst for NH_3-SCR reaction at low temperature

Thermally stable Zr4+, Al3+, and Si4+ cations were incorporated into the lattice of CeO2 nano‐rods (i.e., CeO2‐NR) in order to improve the specific surface area. The undoped and Zr4+, Al3+, and Si4+ doped nano‐rods were used as supports to prepare MnOx/CeO2‐NR, MnOx/CZ‐NR, MnOx/CA‐NR, and MnOx/CS‐NR catalysts, respectively. The prepared supports and catalysts were comprehensively characterized by transmission electron microscopy (TEM), high‐resolution TEM, X‐ray diffraction, Raman and N2‐physisorption analyses, hydrogen temperature‐programmed reduction, ammonia temperature‐programmed desorption, in situ diffuse reflectance infrared Fourier‐transform spectroscopic analysis of the NH3 adsorption, and X‐ray photoelectron spectroscopy. Moreover, the catalytic performance and H2O+SO2 tolerance of these samples were evaluated through NH3‐selective catalytic reduction (NH3‐SCR) in the absence or presence of H2O and SO2. The obtained results show that the MnOx/CS‐NR catalyst exhibits the highest NOx conversion and the lowest N2O concentration, which result from the largest number of oxygen vacancies and acid sites, the highest Mn4+ content, and the lowest redox ability. The MnOx/CS‐NR catalyst also presents excellent resistance to H2O and SO2. All of these phenomena suggest that Si4+ is the optimal dopant for the MnOx/CeO2‐NR catalyst.

Salt-assisted Low Temperature Solid State Synthesis of High Surface Area CoFe_2O_4 Nanoparticles

A novel salt-assisted low temperature solid state method using CoCl2.6H2O, FeCl3.6H2O and NaOH as precursor and using NaCI as a dispersant to synthesize high surface area CoFe2O4 nanoparticles, has been investigated. The effects of the molar ratio of added salt and calcination temperature on the characteristics of the products were investigated by X-ray diffraction （XRD）, transmission electron microscopy （TEM）, vibrating sample magnetometer （VSM） and Brunauer, Emmett and Teller （BET） surface area analysis. Results showed that the introduction of leachable inert inorganic salt as a hard agglomeration inhibitor in the mixture precursor led to the formation of high dispersive CoFe2O4 nanoparticles; and the increase in specific surface area from 28.28 to 73.97 m^2/g, and the saturation magnetization is 84.6 emu/g.

Preparation of transparent yttrium aluminum garnet ceramics by relatively low temperature solid-state reaction

A new preparation method for a highly sinterable Y 2O 3 powder was developed, using the mixture of the powder with Al 2O 3 powder, a transparent yttrium aluminum garnet(YAG) ceramic was prepared at relatively low temperature by a solid state reaction method. Yttrium nitrate was used as a mother salt, and aqueous ammonia was used as a precipitant reagent, the fine and dendritic precursor crystalline was prepared by adding 0.5% ammonium sulfate into the precipitation reaction system. The highly pure and low agglomerated Y 2O 3 powders were obtained by calcinating the precursor at 1 100 ℃, the primary particles are spherical and 60 nm in diameter. The mixture of Y 2O 3 and Al 2O 3 powders was calcinated, and the resulting mixture compact pressed in mold could be sintered to transparency under vacuum at 1 700 ℃. The sintered transparent YAG polycrystalline exhibits a homogeneous microstructure and its transmittance reaches 45% in the visible light region and 70% in the near infrared wavelength region.

Carbonation Reaction of Lithium Hydroxide during Low Temperature Thermal Energy Storage Process

In order to apply lithium hydroxide(LiOH)as a low temperature chemical heat storage material,the carbonation reaction of LiOH and the prevention method are focused in this research.The carbonation of raw LiOH at storage and hydration condition is experimentally investigated.The results show that the carbonation reaction of LiOH with carbon dioxide(CO_(2))is confirmed during the hydration reaction.The carbonation of LiOH can be easily carried out with CO_(2) at room temperature and humidity.LiOH can be carbonated at a humidity range of 10%to 20%,a normal humidity region that air can easily be reached.Furthermore,the carbonation reaction rate has not nearly affected by the increase of reaction temperature.An improved storage method by storing LiOH at a low humidity less than 1.0%can be effectively prevented the carbonation of LiOH.The hydration reaction ratio of LiOH at the improved storage method shows a better result compared to the ordinary storage method.Therefore,the humidity should be carefully controlled during the storage of LiOH before hydration and dehydration reaction when apply LiOH as a low heat chemical storage material.

CO优先氧化反应MnCu/Ce催化剂的制备及性能

采用共浸渍法制备较低Cu含量的MnCu/Ce催化剂,通过XRD、BET、H_(2)-TPR、XPS和CO_(2)-TPD等表征手段对催化剂进行表征,考察催化剂焙烧温度对催化剂结构、性质及其在含有CO_(2)的富氢气氛下对CO优先氧化性能的影响。结果表明,MnCu/Ce催化剂均有Cu/Mn-O-Ce固溶体形成,其中,在焙烧温度600℃制备的催化剂中,Mn与Cu、Ce之间相互作用较强,形成较多三元氧化物固溶体,氧空位/Ce^(3+)含量高,具备良好的CO-Prox活性。此外,对反应条件的考察发现,添加不同分压Ar对催化剂的CO-Prox活性影响较小,气体空速和氧过量系数对催化剂活性影响较大,且反应原料气中CO_(2)的存在对CO-Prox反应有负面影响。氧过量系数为1.2、空速范围为20266-30400 mL/(g·h)时,CO转化率最高,达到94.7%。

Mechanism explanation for SO_2 oxidation rate of Cs-Rb-V series sulfuric acid catalyst at low temperature

The reaction kinetics of SO 2 oxidation on Cs Rb V series sulfuric acid catalyst promoted by alkali salts such as cesium and rubidium was studied. A three step reaction mechanism of SO 2 oxidation was proposed, in which it was assumed that oxidation of quadrivalent vanadium complex was a controlling step. Then, a mechanism model equation was concluded according to the three step reaction mechanism. The SO 2 oxidation rate was measured with a non gradient reactor under the conditions of temperature of 380～520?℃ and space velocity of 3?600～7?200?h -1 . Through calculating with Powell nonlinear regression method, the parameters of model equation were obtained: K 1=0.152?exp(-62?073/ (RT) ), K 2=8.18?exp(-2?384/ (RT) ), K 3=0.221?exp(-18?949/ (RT) ). It was found that the model equation could fit with all the experimental reaction rate data very well. [

Cryoactivated proton-involved redox reactions enable stable-cycling fiber cooper metal batteries operating at-50℃

Fiber-shaped batteries that feature outstanding flexibility,light weight,and wovenability are extremely attractive for powering smart wearable electronic textiles,which further stimulates their demand in extreme environments.However,there are rare reports on ultralow-temperature fiber batteries to date.This is mainly attributed to the poor conductivity of electrodes and freezing of electrolytes that restrain their satisfactory flexible operation in cold environments.Herein,we propose a fiber cooper metal battery consisting of a conductive polyaniline cathode,an anti-freezing Cu(BF4)2+H3PO4electrolyte and an acidresistant copper wire anode,which can withstand various deformations at ultralow temperatures.Impressively,enhanced capacity and cyclic stability can be achieved by cryoactivated abundant reactive sites in the polyaniline,while benefiting from redox reactions with rapid kinetics involving protons rather than copper ions.Consequently,this well-designed polyaniline/Cu fiber battery delivers excellent flexibility without obvious capacity decay after being bent at-30℃,as well as a remarkable discharge capacity of 120.1 mA h g-1and a capacity retention of 96.8%after 2000 cycles at-50℃.The fiber batteries integrated into wearable textiles can power various electronic devices.These performances greatly outperform those of most reported works.Overall,this work provides a promising strategy toward applications of cryogenic wearable energy storage devices.

低温等离子体协同催化CH_(4)-CO_(2)重整反应的研究进展

低温等离子技术的出现为甲烷、二氧化碳重整反应提供了新的思路。阐述了低温等离子体协同催化CH_(4)-CO_(2)重整,并且生成高附加值化学品的合成气(CO和H 2)的基本原理,探究了低温等离子体协同催化CH_(4)-CO_(2)重整反应的反应机理,分析了低温等离子体在协同催化CH_(4)-CO_(2)重整反应中的作用机制,讨论了催化剂的活性组分、载体以及助剂对重整反应的影响,并综述了当前低温等离子协同催化CH_(4)-CO_(2)重整反应过程中的影响因素及存在的问题。

Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge:The performance and absorption mechanism

Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide(SO_(2))and nitrogen oxide(NO_(x))emission control at low temperatures,especially for small and medium-sized coal-fired boilers and furnaces.Herein,phosphorus sludge,an industrial waste from the production process of yellow phosphorus,has been developed to simultaneously eliminate SO_(2)and NO_(x)from coal-fired flue gas.The key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95%can be achieved at a low temperature of 55℃.Further,the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption process.The efficient removal of SO_(2)is attributed to the abundance of iron(Fe^(3+))and manganese(Mn^(2+))in the absorbent.SO_(2)can be rapidly catalyzed and converted to SO_(4)^(2-)by them.The key to NOx removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus,which are then absorbed by water and converted to NO_(3)^(-).Meanwhile,yellow phosphorus is oxidized to phosphoric acid(H_(3)PO_(4)).The spent absorption slurry can be reused through wet process phosphoric acid production,as it contains sulfuric acid(H_(2)SO_(4)),nitric acid(HNO_(3)),and H_(3)PO_(4).Accordingly,this is a technology with broad application prospects.

Ba/Fe双掺LaCoO_(3)热敏陶瓷材料低温离子传输机制研究

为了开发电学性能优异的深低温材料,采用传统高温固态法制备了Ba/Fe双掺杂的LaCoO_(3)负温度系数热敏陶瓷材料,结合XRD、SEM、XPS等测试手段,研究了材料的物相结构、微观形貌、离子价态分布等,并在22—80 K和80—290 K范围内进行了低温电学性能测试。结果表明:双掺杂改性降低了LaCoO_(3)材料的应用温区,ρ(22 K)在1.85×10^(5)—6.94×10^(6)Ω·cm范围内变化,材料常数B(22—100 K)在146.09—162.75 K范围内变化;在深低温环境下,材料的导电机理由80 K以上时的小极化子跳跃导电转变为80 K以下时的双交换导电,导致了材料常数B发生突变。由此证明,该双掺杂热敏陶瓷材料在极低温测试中具有可开发的应用潜力。

低温等离子体协同催化CO_(2)氢化制甲醇的研究

常用的CO_(2)转化技术往往需要高温高压条件,而高温易导致催化剂失活。等离子体技术因操作条件简单、能量成本低等优点成为CO_(2)催化转化的新型应用技术。甲醇作为重要的化工原料和能源被广泛应用,利用等离子体技术在室温、常压下将CO_(2)转化为高附加值产物甲醇被热点研究。通过介绍等离子体催化体系驱动CO_(2)氢化制甲醇的研究进展,从催化剂、反应条件等方面综述影响反应效率的因素。同时,综述低温等离子体催化CO_(2)加氢制甲醇反应的机理,给出了CO_(2)氢化制甲醇的未来重点研究方向。CO_(2)加氢气制甲醇不仅可以减少CO_(2)排放,且生成物可以有效缓解我国当前能源及化工原材料缺口,具有现实意义和广阔的研究前景。

低温共沉淀法合成多孔CoFe LDH纳米片电催化剂

通过低温共沉淀技术合成了多孔CoFe层状双金属氢氧化物(CoFe LDH)纳米片。运用X射线衍射(XRD)、X射线光电子能谱(XPS)、扫描电镜(SEM)、透射电镜(TEM)等手段对产物的物相、组成及微观形貌进行了表征,并探讨了铁离子(Fe3+)含量对CoFe LDH纳米结构生长行为的影响,考察了制备的产物作为电催化剂在电解水析氧反应中的性能。结果表明,Fe3+的加入可以有效调节产物的形貌、结晶度和孔道结构。在合适的Co与Fe比例条件下,制备的CoFe LDH可形成多孔纳米片,且增大了总孔体积,增加了表面活性位点。同时,结晶CoFe LDH纳米片可促进Co和Fe离子间的电荷转移行为,从而提高产物的电催化活性。对于电解水析氧反应,当电流密度为10 mA/cm2时,结晶Co0.67Fe0.33 LDH多孔纳米片所需的过电势仅为291 mV,Tafel斜率为33 mV/dec,并展现出良好的循环稳定性。

绿色MOFs基固体酸低温催化制备生物柴油

生物柴油是重要的可再生能源,有希望代替化石燃料满足世界的能源需求。开发具有高Lewis酸性位点的多孔材料用于催化酯化反应制备生物柴油是当下的热门领域。以无溶剂法,通过生物质基2,5-呋喃二甲酸(FDCA)与氧氯化锆的简易组装,制备了介孔-金属有机杂化物FDCA-Zr,并通过油酸与甲醇进行酯化反应生成脂肪酸甲酯(FAME)的反应过程验证了其催化活性。采用XRD、FT-IR、BET、SEM、TEM、STEM-Mapping、热重分析、吡啶红外等方法对FDCA-Zr进行了详细的结构和性质分析。结果表明:FDCA-Zr具有良好的颗粒尺寸和优秀的催化性能,与传统的固体酸催化剂以及液体酸催化剂相比,在长烷基链脂肪酸的酯化反应中表现出相当或优越的催化效果,FAME的收率可达到98%。此外,FDCA-Zr在连续循环使用过程中结构稳定,在6次循环后FAME的收率仍保持在90%,重复利用性良好。

Doping effect of rare earth metal ions Sm^(3+),Nd^(3+)and Ce^(4+)on denitration performance of MnO_(x) catalyst in low temperature NH_(3)-SCR reaction

The MnXO_(x) catalysts(i.e.,MnSmO_(x),MnNdO_(x),MnCeO_(x)) were prepared by reverse co-precipitation method and used for NH_(3)-SCR reaction.It is found that MnCeO_(x) catalyst presents the best low tempe rature catalytic activity(higher than 90% NO_(x) conversion in the te mperature range from 125 to 225℃)and excellent H_(2)O+SO_(2) resistance.In order to explore the reason for this result,the characterization of X-ray diffraction(XRD),Raman spectroscopy,Brunauer-Emmett-Teller(BET),H_(2)-temperature programmed reduction(H_(2)-TPR),NH_(3)-temperature programmed desorption(NH_(3)-TPD),X-ray photoelectron spectroscopy(XPS) and in situ diffuse reflaxions infrared Fourier transformations spectroscopy(DRIFTS) were conducted.The obtained results suggest that MnCeO_(x) catalyst shows the largest amount of acid sites and the best reducibility among these MnXO_(x) catalysts.Besides,Ce^(4+) doping inhibits the crystallization of MnO_(x) catalyst and shows the largest specific surface area.Finally,in situ DRIFTS experiments reveal that NH_(3)-SCR reaction over MnCeO_(x) catalyst follows both Langmuir-Hinshelwood(LH) and Eley-Rideal(E-R) mechanisms,which is through "fast SCR" reaction.

Realizing Complete Solid-Solution Reaction to Achieve Temperature Independent LiFePO_(4) for High Rate and Low Temperature Li-Ion Batteries

The lithium iron phosphate battery(LiFePO4 or LFP)does not satisfactorily deliver the necessary high rates and low temperatures due to its low Li+diffusivity,which greatly limits its applications.The solid-solution reaction,compared with the traditional two-phase transition,needs less energy,and the lithium ion diffusivity is also higher,which makes breaking the barrier of LFP possible.However,the solid-solution reaction in LFP can only occur at high rates due to the lattice stress caused by the bulk elastic modulus.Herein,pomegranate-like LFP@C nanoclusters with ultrafine LFP@C subunits(8 nm)(PNCsLFP)were synthesized.Using in situ X-ray diffraction,we confirmed that PNCsLFP can achieve complete solid-solution reaction at the relatively low rate of 0.1C which breaks the limitation of low lithium ion diffusivity of the traditional LFP and frees the lithium ion diffusivity from temperature constraints,leading to almost the same lithium ion diffusivities at room temperature,0,−20,and−40℃.The complete solid-solution reaction at all rates breaks the shackles of limited lithium ion diffusivity on LFP and offers a promising solution for next-generation lithium ion batteries with high rate and low temperature applications.

不同麻醉深度指数下拔管在扁桃体低温等离子射频消融术患儿中的应用效果比较

目的:比较不同麻醉深度指数(NT值)下拔管在扁桃体低温等离子射频消融术患儿中的应用效果。方法:选取2021年7月至2022年4月于该院行扁桃体低温等离子射频消融术的76例患儿进行前瞻性研究,按照随机数字表法将其分为对照组和观察组各38例。两组均行气管插管全身麻醉,对照组于NT值为95~100时拔管,观察组于NT值为80~94时拔管。比较两组不同时间[停止麻醉维持即刻(T_(0))、拔管后即刻(T_(1))、拔管后10 min(T_(2))]血流动力学指标(心率、平均动脉压、呼吸频率)水平、不同时间(拔管前、拔管后30 min)应激指标[皮质醇(Cor)、肾上腺素(E)]水平、不同时间(T_(0)、T_(1)、T_(2))局部脑氧饱和度(rSO_(2))水平和不良反应发生率。结果:T_(1)、T_(2)时,两组平均动脉压、心率、呼吸频率均高于T_(0)时,但观察组低于对照组,差异有统计学意义(P<0.05);拔管后30 min,两组Cor、E水平均高于拔管前,但观察组低于对照组,差异有统计学意义(P<0.05);T_(0)、T_(1)、T_(2)时,两组rSO_(2)水平比较,差异均无统计学意义(P>0.05);观察组不良反应发生率为5.26%(2/38),低于对照组的21.05%(8/38),差异有统计学意义(P<0.05)。结论:NT值为80~94时拔管应用于扁桃体低温等离子射频消融术患儿可改善血流动力学指标和应激指标水平,降低不良反应发生率,效果优于NT值为80~94时拔管。

无铬CO高温变换催化剂的研究Ⅱ.过渡元素对高变催化剂结构与性能的影响

通过ＸＲＤ，ＢＥＴ和ＸＰＳ表征及反应性能测定表明，铁系高变催化剂中加入的过渡元素能够进入Ｆｅ３Ｏ４晶格形成固溶体，并使催化剂的晶胞参数随着加入元素离子半径的增大而增大，晶粒度明显变小，比表面积增大，起到铬的作用，催化剂的活性和热稳定性提高．发现部分过渡元素具有富集ＯＨ－的特性，使催化剂在较低的汽／气比条件下具有较高的催化活性．研制成功的Ｂ１２１型无铬高变催化剂性能达到铁铬系高变催化剂的技术指标．

无铬CO高温变换催化剂的研究 Ⅰ.氧化铬对高变催化剂结构与性能的影响

通过ＸＲＤ，ＢＥＴ和ＸＰＳ表征及反应活性测定表明，ＣＯ高温变换催化剂中加入的助剂ＣｒＯ３在制备及还原过程中，能进入Ｆｅ３Ｏ４晶格，使晶胞参数增大、晶粒度变小、分散度提高、比表面积和孔容积增大、孔结构改善而提高催化剂活性和稳定性．加入的ＣｒＯ３有７６％以Ｃｒ３＋形态存在于尖晶石的正八面体空隙中，２４％以Ｃｒ６＋形态存在于正八面体和正四面体空隙中．氧化铬不仅起到结构助剂作用，可能还起到电子助剂作用．加入的Ｃｒ２Ｏ３不进入Ｆｅ３Ｏ４晶格而以独立相存在，不起助剂作用．