Silica-modified Pt/TiO_(2) catalysts with tunable suppression of strong metal-support interaction for cinnamaldehyde hydrogenation

Tuning Strong Metal-support Interactions(SMSI)is a key strategy to obtain highly active catalysts,but conventional methods usually enable TiO_(x) encapsulation of noble metal components to minimize the exposure of noble metals.This study demonstrates a catalyst preparation method to modulate a weak encapsulation of Pt metal nanoparticles(NPs)with the supported TiO_(2),achieving the moderate suppression of SMSI effects.The introduction of silica inhibits this encapsulation,as reflected in the characterization results such as XPS and HRTEM,while the Ti^(4+) to Ti^(3+) conversion due to SMSI can still be found on the support surface.Furthermore,the hydrogenation of cinnamaldehyde(CAL)as a probe reaction revealed that once this encapsulation behavior was suppressed,the adsorption capacity of the catalyst for small molecules like H_(2) and CO was enhanced,which thereby improved the catalytic activity and facilitated the hydrogenation of CAL.Meanwhile,the introduction of SiO_(2) also changed the surface structure of the catalyst,which inhibited the occurrence of the acetal reaction and improved the conversion efficiency of C=O and C=C hydrogenation.Systematic manipulation of SMSI formation and its consequence on the performance in catalytic hydrogenation reactions are discussed.

高内相乳液模板法制备P(BMA-co-MMA)多孔树脂及其吸油性能

采用高内相乳液模板法,以甲基丙烯酸丁酯(BMA)和甲基丙烯酸甲酯(MMA)为单体、二乙烯苯(DVB)为交联剂、失水山梨醇油酸酯(Span 80)为乳化剂、偶氮二异庚腈(AVBN)为引发剂,合成了可压缩、高弹性的P(BMA-co-MMA)多孔吸油树脂。采用红外光谱和扫描电镜对多孔树脂的结构进行表征,并测试了多孔树脂的力学性能,考察了单体配比和表面活性剂用量对树脂吸油性能的影响,评价了其油水分离性能。结果表明,以m(BMA):m(MMA)=7:3,Span 80用量占单体总质量的16.67%制备的P(BMA-co-MMA)多孔树脂的吸油性能最佳,对二氯甲烷的吸附量高达51.95 g/g,保油率可达93%以上。此外,该多孔树脂具有良好的超亲油疏水性,水接触角(WCA)可达到143°,油接触角接近0°,能够在20 s内完全吸附水中的甲苯,有望在油水分离方面得到应用。

Ink formulation, scalable applications and challenging perspectives of screen printing for emerging printed microelectronics

Screen printing is regarded as a highly competitive manufacture technology for scalable and fast fabrication of printed microelectronics, owing to its advanced merits of low-cost, facile operability and scalability.However, its large-scale application in printed microelectronics is still limited by screen printing functional ink. In this review, we summarize the recent advances of ink formation, typical scalable applications, and challenging perspectives of screen printing for emerging printed microelectronics. Firstly, we introduce the major mechanism of screen printing and the formation of different organic-and aqueous-based inks by various solvents and binders. Next, we review the most widely used applications of screen printing technique in micro-batteries, micro-supercapacitors and micro-sensors, demonstrative of wide applicability.Finally, the perspectives and future challenges in the sight of screen printing are briefly discussed.

Aqueous high-voltage all 3D-printed micro-supercapacitors with ultrahigh areal capacitance and energy density

With the rapid development of integrated and miniaturized electronics,the planar energy storage devices with high capacitance and energy density are in enormous demand.Hence,the advanced manufacture and fast fabrication of microscale planar energy units are of great significance.Herein,we develop aqueous planar micro-supercapacitors(MSCs) with ultrahigh areal capacitance and energy density via an efficient all-3 D-printing strategy,which can directly extrude the active material ink and gel electrolyte onto the substrate to prepare electrochemical energy storage devices.Both the printed active carbon/exfoliated graphene(AC/EG) electrode ink and electrolyte gel are highly processable with outstanding conductivity(~97 S cm^(-1) of electrode;-34.8 mS cm^(-1) of electrolyte),thus benefiting the corresponding shaping and electrochemical performances.Furthermore,the 3 D-printed symmetric MSCs can be operated stably at a high voltage up to 2.0 V in water-in-salt gel electrolyte,displaying ultrahigh areal capacitance of2381 mF cm^(-2) and exceptional energy density of 331 μWh cm^(-2),superior to previous printed micro energy units.In addition,we can further tailor the integrated 3 D-printed MSCs in parallel and series with various voltage and current outputs,enabling metal-free interconnection.Therefore,our all-3 D-printed MSCs place a great potential in developing high-power micro-electronics fabrication and integration.

Low-temperature and high-voltage planar micro-supercapacitors based on anti-freezing hybrid gel electrolyte

Micro-supercapacitors(MSCs)are considered as highly competitive power sources for miniaturized electronics.However,narrow voltage window and poor anti-freezing properties of MSCs in conventional aqueous electrolytes lead to low energy density and limited environmental adaption.Herein,we report the construction of low-temperature and high-energy-density MSCs based on anti-freezing hybrid gel electrolytes(HGE)through introducing ethylene glycol(EG)additives into aqueous LiCl electrolyte.Since EG partially destroys hydrogen bond network among water molecules,the HGE exhibits maximum electrochemical stability window of 2.7 V and superior anti-freezing features with a glass transition temperature of-62.8℃.Further,the optimized MSCs using activated carbon microelectrodes possess impressive volumetric capacitance of 28.9 F cm^(-3)and energy density of 10.3 mWh cm^(-3)in the voltage of 1.6 V,2.6 times higher than MSCs tested in 1.2 V.Importantly,the MSCs display 68.3%capacitance retention even at-30℃ compared to the value at 25℃,and ultra-long cyclability with 85.7%of initial capacitance after 15,000 times,indicating extraordinary low-temperature performance.Besides,our devices offer favorable flexibility and modular integration.Therefore,this work provides a general strategy of realizing flexible,safe and anti-freezing microscale power sources,holding great potential towards subzero-temperature microelectronic applications.

The steady and vibrating statuses of tulip tree leaves in wind

The study of tree leaf aerodynamics is useful to tree protection, solar panel design and development of new power generation technology. 73 tulip leaves were tested in suspended condition and with front as well as back surface of the lamina facing wind. Three types of vibrating statuses, two types of steady statuses, and five critical wind speeds were observed. The existence probabilities of the statuses and criticals, the probability density distribution of every critical over the range of wind speed 0-27 m/s, and the expected values of the criticals were obtained by statistics. The critical Reynolds number, defined by critical wind speed and lamina length, shows an increasing trend with increasing the lamina area or length to width ratio of the lamina, but it shows no trend of increase or decrease with increasing the length ratio of petiole to lamina.

2.4 V ultrahigh-voltage aqueous MXene-based asymmetric micro-supercapacitors with high volumetric energy density toward a self-sufficient integrated microsystem

Two-dimensional MXenes are key high-capacitance electrode materials for micro-supercapacitors(MSCs)catering to integrated microsystems.However,the narrow electrochemical voltage windows of conventional aqueous electrolytes(≤1.23 V)and symmetric MXene MSCs(typically≤0.6 V)substantially limit their output voltage and energy density.Highly concentrated aqueous electrolytes exhibit lower water molecule activity,which inhibits water splitting and consequently widens the operating voltage window.Herein,we report ultrahigh-voltage aqueous planar asymmetric MSCs(AMSCs)based on a highly concentrated LiCl-gel quasi-solid-state electrolyte with MXene(Ti3C2Tx)as the negative electrode and MnO_(2) nanosheets as the positive electrode(MXene//MnO_(2)-AMSCs).The MXene//MnO_(2)-AMSCs exhibit a high voltage of up to 2.4 V,attaining an ultrahigh volumetric energy density of 53 mWh cm−3.Furthermore,the in-plane geometry and the quasi-solid-state electrolyte enabled excellent mechanical flexibility and performance uniformity in the serially/parallel connected packs of our AMSCs.Notably,the MXene//MnO_(2)-AMSC-based integrated microsystem,in conjunction with solar cells and consumer electronics,could efficiently realize simultaneous energy harvesting,storage,and conversion.The findings of this study provide insights for constructing high-voltage aqueous MXene-based AMSCs as safe and self-sufficient micropower sources in smart integrated microsystems.

中国植物性饮食结构调整具有显著的耕地资源效应

Food systems are already a major contributor to land degradation,and changes in global diets will exacerbate this situation[1].Population growth and affluent dietary patterns result in changes in land demand and land-use patterns,and up to 40% of global arable land and more than 30% of global food-crop production are used for animal feed[2].Furthermore,food-feed competition can result in an inadequate food supply[3].

Targeting BCL9/BCL9L enhances antigen presentation by promoting conventional type 1 dendritic cell(cDC1)activation and tumor infiltration

Conventional type 1 dendritic cells(cDC1)are the essential antigen-presenting DC subset in antitumor immunity.Suppressing B-cell lymphoma 9 and B-cell lymphoma 9-like(BCL9/BCL9L)inhibits tumor growth and boosts immune responses against cancer.However,whether oncogenic BCL9/BCL9L impairs antigen presentation in tumors is still not completely understood.Here,we show that targeting BCL9/BCL9L enhanced antigen presentation by stimulating cDC1 activation and infiltration into tumor.Pharmacological inhibition of BCL9/BCL9L with a novel inhibitor hsBCL9z96 or Bcl9/Bcl9l knockout mice markedly delayed tumor growth and promoted antitumor CD8^(+)T cell responses.Mechanistically,targeting BCL9/BCL9L promoted antigen presentation in tumors.This is due to the increase of cDC1 activation and tumor infiltration by the XCL1-XCR1 axis.Importantly,using single-cell transcriptomics analysis,we found that Bcl9/Bcl9l deficient cDC1 were superior to wild-type(WT)cDC1 at activation and antigen presentation via NF-κB/IRF1 signaling.Together,we demonstrate that targeting BCL9/BCL9L plays a crucial role in cDC1-modulated antigen presentation of tumor-derived antigens,as well as CD8^(+)T cell activation and tumor infiltration.Targeting BCL9/BCL9L to regulate cDC1 function and directly orchestrate a positive feedback loop necessary for optimal antitumor immunity could serve as a potential strategy to counter immune suppression and enhance cancer immunotherapy.

高熵MXenes在储能和催化中的应用展望

In less than a decade,MXenes,a family of two-dimensional(2D)transition-metal carbide/nitrides,have pushed the boundaries of electrochemical performance attained by various energy storage devices[1].The all-round excellent achievements of MXene so far are reminiscent of the "graphene era" thanks to their unique features,such as hydrophilicity,conductivity,and redox pseudocapacitance.The functions of MXene could be tuned by modifying the surface functional groups using various chemical treatments like alkalization by KOH or molten-salt synthesis[1].In addition to the functional groups,various permutations and combinations of multiple transition metals are also possible which further enrich the properties of MXenes compared to mono-transition-metal MXenes(MTMs)[1]and boost the structural and oxidation stability for energy storage and catalysis.

Advancing MXene-based integrated microsystems with microsupercapacitors and/or sensors:Rational design,key progress,and challenging perspectives

The escalating demand for micro/nano-sized devices,such as micro/nano-robots,intelligent portable/wearable microsystems,and implantable medical microdevices,necessitates the expeditious development of integrated microsystems incorporating energy conversion,storage,and consumption.Critical bottlenecks in microscale energy storage/sensors and their integrated systems are being addressed by exploring new technologies and new materials,e.g.,MXene,holding great potential for developing lightweight and deformable integrated microdevices.This review summarizes the latest progress and milestones in the realization of MXene-based micro-supercapacitors(MSCs)and sensor arrays,and thus discusses the design fundamentals and key advancements of MXene-based energy conversion-storageconsumption integrated microsystems.Finally,we outline the key challenges in fabricating MXenebased MSCs/sensors and their self-powered integrated microsystems,which is crucial for their practical applications.Particularly,we illuminate viable solutions to such unsolved issues and highlight the exciting opportunities.

Research on Gesture Recognition Based on Multialgorithm Fusion

Aiming at people with hearing and speaking obstacles,this paper pro-poses a multialgorithm fusion for gesture recognition.This paper aims to more clearly distinguish easily confused gestures in gesture recognition and improve gesture recognition accuracy by integrating lip-reading recognition.For gesture recognition,this paperfirst performs skin color processing and segmentation on the hand area of the collected video sequence and detects the hand feature points by calling the hand key point model.The extracted gesture features are trained and recognized by the support vector machine algorithm.For lip reading recognition,this paperfirst uses the AdaBoost algorithm to detect and track key points on the collected video sequence,locate the lips,extract the key points of the lips through a convolutional neural network,and input the extracted key point feature sequence into BiLSTM to extract semantic information.The fusion of gesture recognition and lip reading recognition algorithms using the YOLOV5 model can effectively improve the accuracy of gesture recognition.Through experimental verification,the recognition rate can be increased from 89.4%to 94.3%.

The potential of engineered multifunctional quantum dots for macrophage theranostics

Macrophages play important roles in tissue repair,inflammation,and the progression of various diseases.Imaging and tracking macrophage cells in vitro and in vivo can reveal the location and movement of macrophages in tissues and animals,which is critical to understanding macrophage functions in different diseases.1 Macrophages can generally be divided into the following two phenotypes based on their physiological functions:proinflammatory M1 macrophages and alternatively activated M2 macrophages,both of which are closely related to the development and progression of various diseases.A promising methodology for disease therapy is the modulation of macrophage phenotypes,which can reverse disease states and metabolic processes.Therefore,engineering nanoparticles that combine the advantages of imaging and therapy may offer novel strategies for macrophage theranostics.

高效体积排阻色谱法定量检测口蹄疫疫苗中146S的疫苗预处理方法

旨在建立一种口蹄疫灭活病毒疫苗的处理方法,去除尺寸排阻色谱法(HPSEC)检测146S抗原过程中的杂质干扰,获得最佳的检测信号并实现146S抗原含量的准确测定。分别考察了超速离心法、PEG沉淀法、核酸酶消化法对两批疫苗样品中的HPSEC检测干扰杂质的去除效果。在优化条件下,超速离心法处理后146S检测结果分别为7.1、7.6 μg/mL,PEG沉淀法为9.7、10.4 μg/mL;酶消化法处理后的检测值最高,分别为10.5、10.4 μg/mL,且杂质去除完全、处理速度快、操作条件温和。通过响应面法确定最优酶消化处理条件如下:200 μL水相中添加终浓度421 U/mL的Benzonase,25.1 ℃下反应1.29 h。在该最优条件下,对4家企业各3种不同血清型共12批疫苗样品进行146S含量检测,结果表明建立的方法对不同疫苗均有良好适用性,且重复性好(RSD<5.3%,n=3)。通过该处理方法,解决了杂质对146S定量检测的干扰,扩大了HPSEC检测技术的应用范围,进一步确保了检测结果的准确可靠。

流动化学在卤化反应中的应用

有机物的卤化反应是有机合成中最重要的转化之一.传统釜式卤化反应存在高放热及选择性差等问题,且卤化试剂一般具有毒性和腐蚀性.流动化学在传质和传热方面具有显著优势,可精确控制反应温度及试剂用量,并且可在线淬灭危险试剂,避免其暴露.按有机化合物卤化反应分类,系统地归纳了流动化学在氟化反应、氯化反应、溴化反应和碘化反应中的应用进展,并展望了其发展趋势.

磷酸酯类前药的合成方法与应用

磷酸酯类前药与原药相比,不仅能够提高药物靶向性、稳定性和生物利用度,减少药物毒副作用,还能掩蔽药物不适气味、提高水溶性从而改善给药途径。含羟基药物的磷酸酯化是该类药物前药设计的重要方法之一。本文根据中心磷原子的价态和化合物结构进行分类,综述了各种P(Ⅴ)四配位分子、P(Ⅲ)三配位分子和H-亚磷酸酯类化合物作为磷酸酯化试剂在磷酸酯类前药合成方法中的研究进展,并阐述了这些磷酸酯类药物的应用,最后总结了各类磷酸酯化试剂的优势与局限,并结合连续流反应技术应用案例展望了其发展趋势。

Cell-Mediated Immunity Imbalance in Patients with Intrahepatic Cholestasis of Pregnancy

Decidual lymphocytes may mediate fetal trophoblast recognition and regulate maternal immune reaction and play an essential role in the maintenance of normal pregnancy. The aim of this study was to compare the percentage of T cells, natural killer （NK） cells and natural killer T （NKT） cells within decidual parietalis of normal pregnant controls （NP） and patients with intraheptic cholestasis of pregnancy （ICP）, and to investigate the production of interleukin-4 （IL-4）, interferon-γ （IFN-γ） in the culture supernatant of decidual parietalis mononuclear cells （DPMCs）. Compared with controls, the decidua parietalis from ICP were characterized with significant increased percentages of CD3^＋CD56^＋ cells, CD3^＋CD56^＋ cells, CD56^＋CD16＋ cells, CD56^＋CD16^＋ cells, CD56^＋NKG2D＋ ceils, and the significant decreased percentages of CD3^＋ cells, CD3^＋CD4^＋ cells. There were no differences found for the percentage of CD3^＋CD8^＋ cells, CD56^＋NKG2A^＋ cells between control and study group. In addition, the enhanced concentration of IFN-γ was presented in culture supernatant of DPMCs from ICP. It was suggested that the increased NK cells, NKT cells and the decreased T cells in the decidual parietalis and over-secretion of IFN-γ could be correlated with the pathophysiology of ICP patients. Cellular ＆ Molecular Immunology. 2007;4（1）：71-75.

Halogen effects on phenylethynyl palladium(Ⅱ) complexes for living polymerization of isocyanides: a combined experimental and computational investigation

Phenylethynyl palladium(Ⅱ) complexes have proven to be effective catalysts for coordination polymerization of isocyanides. In this work, two new phenylethynyl palladium(Ⅱ) initiators bearing bromide(1b) and iodide(1c) were synthesized and applied for living polymerization of aryl and alkyl isocyanides. The coordinated halogen anions can significantly influence the kinetics of polymerization, with the observed order of reaction rates being 1c(Ⅰ)>1 b(Br)>1a(Cl). Impressively, 1c not only accelerates the reaction rate in both the initiation stage and propagation stage, but also can polymerize less active monomers that cannot be reacted by 1a. DFT calculations were then employed to understand the detailed mechanism and the halogen effects in this insertion polymerization process.

Dynamic Variations in Brain Glycogen are Involved in Modulating Isoflurane Anesthesia in Mice

General anesthesia severely affects the metabolites in the brain.Glycogen,principally stored in astrocytes and providing the short-term delivery of substrates to neurons,has been implicated as an affected molecule.However,whether glycogen plays a pivotal role in modulating anesthesia-arousal remains unclear.Here,we demonstrated that isoflurane-anesthetized mice exhibited dynamic changes in the glycogen levels in various brain regions.Glycogen synthase(GS)and glycogen phosphorylase(GP),key enzymes of glycogen metabolism,showed increased activity after isoflurane exposure.Upon blocking glycogenolysis with 1,4-dideoxy-1,4-imino-Darabinitol(DAB),a GP antagonist,we found a prolonged time of emergence from anesthesia and an enhancedδfrequency in the EEG(electroencephalogram).In addition,augmented expression of glycogenolysis genes in glycogen phosphorylase,brain(Pygb)knock-in(PygbH11/H11)mice resulted in delayed induction of anesthesia,a shortened emergence time,and a lower ratio of EEG-δ.Our findings revealed a role of brain glycogen in regulating anesthesiaarousal,providing a potential target for modulating anesthesia.

Detection of Picric Acid by Terpy-Based Metallo- Supramolecular Fluorescent Coordination Polymers in Aqueous Media

The synthesis of two linear terpy-based metallo-supramolecular fluorescent coordination polymers through 1 ： 1 complexation of Zn^2＋ and Cd^2＋ ions with ditopic terpyridine ligand was reported. The dispersibility of P1 and P2 was significantly improved in organic solvent and water through the introduction of hydrophilic oligo-ethyoxy side chain. Two polymers displayed yellow light emission both in solution and the solid state due to the intra-ligand charge transfer （ILCT） between the d^10 metal ions and the conjugated spacer unit. These coordination polymers were explored as fluorescent chemosensors for detecting picric acid in aqueous media, displaying high sensitivity and good selectivity. In addition, test strips were prepared from these polymers and exhibited the practical potential of detecting the NACs pollutants in the outdoor water for public safety and security.