Encapsulated Ni-Co alloy nanoparticles as efficient catalyst for hydrodeoxygenation of biomass derivatives in water

Catalytic hydrodeoxygenation(HDO)is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels,but highly challenging due to the lack of highly efficient nonprecious metal catalysts.Herein,we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst.The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100%conversion efficiency and selectivity under mild reaction conditions,surpassing the reported high performance nonprecious HDO catalysts.Impressively,our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100%conversion efficiency and over 90%selectivity.Importantly,our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O,and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs.The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.

Effects of electron-and hole-current hysteresis on trap characterization in organo-inorganic halide perovskite

Charge trap density and carrier mobility of perovskite materials are the critical properties of perovskite solar cells.The space charge limited current(SCLC)method,which measures a dark current–voltage(I-V)curve of a single-carrier device has found extensive use for studying the trap density and charge carrier mobility in perovskite materials.Herein,it was found that the electron-and hole-current in organo-lead perovskite-based single-carrier device undergoes significant hysteresis under forward and reverse scanning due to the mobile ions.In addition,it was also observed that measuring history has a detrimental effect on hysteresis resulting in possible overestimation or underestimation of the extracted electrical values from the SCLC measurement.In the forward/reverse scanning process,the mobile ionic defects enhance/shield the charge in the traps due to ionic charging/discharging,thereby increasing/reducing the interface barrier and net charge in the I-V scanning,which in turn affects the determination of transport properties of the carrier.These results raise quite a few doubts over the direct application of classical SCLC measurements for the accurate characterization of intrinsic transport properties of the mixed ionicelectronic perovskite.

Self-adjuvant Astragalus polysaccharide-based nanovaccines for enhanced tumor immunotherapy:a novel delivery system candidate for tumor vaccines

The study of tumor nanovaccines(NVs)has gained interest because they specifically recognize and eliminate tumor cells.However,the poor recognition and internalization by dendritic cells(DCs)and insufficient immunogenicity restricted the vaccine efficacy.Herein,we extracted two molecular-weight Astragalus polysaccharides(APS,12.19 k D;APSHMw,135.67 k D)from Radix Astragali and made them self-assemble with OVA257–264directly forming OVA/APS integrated nanocomplexes through the microfluidic method.The nanocomplexes were wrapped with a sheddable calcium phosphate layer to improve stability.APS in the formed nanocomplexes served as drug carriers and immune adjuvants for potent tumor immunotherapy.The optimal APS-NVs were approximately 160 nm with uniform size distribution and could remain stable in physiological saline solution.The FITC-OVA in APS-NVs could be effectively taken up by DCs,and APS-NVs could stimulate the maturation of DCs,improving the antigen cross-presentation efficiency in vitro.The possible mechanism was that APS can induce DC activation via multiple receptors such as dectin-1 and Toll-like receptors 2 and 4.Enhanced accumulation of APS-NVs both in draining and distal lymph nodes were observed following s.c.injection.Smaller APS-NVs could easily access the lymph nodes.Furthermore,APS-NVs could markedly promote antigen delivery efficiency to DCs and activate cytotoxic T cells.In addition,APS-NVs achieve a better antitumor effect in established B16-OVA melanoma tumors compared with the OVA+Alum treatment group.The antitumor mechanism correlated with the increase in cytotoxic T cells in the tumor region.Subsequently,the poor tumor inhibitory effect of APS-NVs on the nude mouse model of melanoma also confirmed the participation of antitumor adaptive immune response induced by NVs.Therefore,this study developed a promising APS-based tumor NV that is an efficient tumor immunotherapy without systemic side effects.

Self-Adaptive Control System for Additive Manufacturing Using Double Electrode Micro Plasma Arc Welding

Wire arc additive manufacturing(WAAM)has been investigated to deposit large-scale metal parts due to its high deposition efficiency and low material cost.However,in the process of automatically manufacturing the high-quality metal parts by WAAM,several problems about the heat build-up,the deposit-path optimization,and the stability of the process parameters need to be well addressed.To overcome these issues,a new WAAM method based on the double electrode micro plasma arc welding(DE-MPAW)was designed.The circuit principles of different metal-transfer models in the DE-MPAW deposition process were analyzed theoretically.The effects between the parameters,wire feed rate and torch stand-off distance,in the process of WAAM were investigated experimentally.In addition,a real-time DE-MPAW control system was developed to optimize and stabilize the deposition process by self-adaptively changing the wire feed rate and torch stand-off distance.Finally,a series of tests were performed to evaluate the control system’s performance.The results show that the capability against interferences in the process of WAAM has been enhanced by this self-adaptive adjustment system.Further,the deposition paths about the metal part’s layer heights in WAAM are simplified.Finally,the appearance of the WAAM-deposited metal layers is also improved with the use of the control system.

Multicut L-Shaped Algorithm for Stochastic Convex Programming with Fuzzy Probability Distribution

Two-stage problem of stochastic convex programming with fuzzy probability distribution is studied in this paper. Multicut L-shaped algorithm is proposed to solve the problem based on the fuzzy cutting and the minimax rule. Theorem of the convergence for the algorithm is proved. Finally, a numerical example about two-stage convex recourse problem shows the essential character and the efficiency.

The chemerin-CMKLR1 axis in keratinocytes impairs innate host defense against cutaneous Staphylococcus aureus infection

The skin is the most common site of Staphylococcus aureus infection,which can lead to various diseases,including invasive and life-threatening infections,through evasion of host defense.However,little is known about the host factors that facilitate the innate immune evasion of S.aureus in the skin.Chemerin,which is abundantly expressed in the skin and can be activated by proteases derived from S.aureus,has both direct bacteria-killing activity and immunomodulatory effects via interactions with its receptor CMKLR1.Here,we demonstrate that a lack of the chemerin/CMKLR1 axis increases the neutrophil-mediated host defense against S.aureus in a mouse model of cutaneous infection,whereas chemerin overexpression,which mimics high levels of chemerin in obese individuals,exacerbates S.aureus cutaneous infection.Mechanistically,we identified keratinocytes that express CMKLR1 as the main target of chemerin to suppress S.aureus-induced IL-33 expression,leading to impaired skin neutrophilia and bacterial clearance.CMKLR1 signaling specifically inhibits IL-33 expression induced by cell wall components but not secreted proteins of S.aureus by inhibiting Akt activation in mouse keratinocytes.Thus,our study revealed that the immunomodulatory effect of the chemerin/CMKLR1 axis mediates innate immune evasion of S.aureus in vivo and likely increases susceptibility to S.aureus infection in obese individuals.

The kinase p38αfunctions in dendritic cells to regulate Th2-cell differentiation and allergic inflammation

Dendritic cells(DCs)play a critical role in controlling T helper 2(Th2)cell-dependent diseases,but the signaling mechanism that triggers this function is not fully understood.We showed that p38αactivity in DCs was decreased upon HDM stimulation and dynamically regulated by both extrinsic signals and Th2-instructive cytokines.p38α-specific deletion in cDC1s but not in cDC2s or macrophages promoted Th2 responses under HDM stimulation.Further study showed that p38αin cDC1s regulated Th2-cell differentiation by modulating the MK2−c-FOS−IL-12 axis.Importantly,crosstalk between p38α-dependent DCs and Th2 cells occurred during the sensitization phase,not the effector phase,and was conserved between mice and humans.Our results identify p38αsignaling as a central pathway in DCs that integrates allergic and parasitic instructive signals with Th2-instructive cytokines from the microenvironment to regulate Th2-cell differentiation and function,and this finding may offer a novel strategy for the treatment of allergic diseases and parasitic infection.

Dual-miRNA-Propelled Three-Dimensional DNA Walker for Highly Specific and Rapid Discrimination of Breast Cancer Cell Subtypes in Clinical Tissue Samples

Accurate discrimination of cell subtypes at the molecular level is especially important for cancer diagnosis,but no current method allows rapid and precise detection of breast cancer subtypes.Herein,we developed an elegant DNA walker for direct and rapid differentiation of breast cancer cell subtypes via detection of dual-miRNAs in clinical tissue samples.This DNA nanomachine can be specifically initiated by endogenous miR-21 and miR-31,and the sensitivity was dramatically improved due to the DNAzyme-mediated signal amplification.This DNA walker enabled rapid detection of double miRNA characteristics in different breast cell lines and also distinguished the fluctuations in a single cell.Applications of this DNAzyme-based nanomachine in vivo and in clinical samples were demonstrated for efficient detection of breast cancer subtypes,making the method generally applicable for precise management of cancers.

Interfacial engineering of metallic rhodium by thiol modification approach for ambient electrosynthesis of ammonia

Here we report a vapor-phase reaction approach to fabricate rhodium(I)-dodecanethiol complex coated on carbon fiber cloth(Rh(I)-SC_(12)H_(25)/CFC),followed by low-temperature pyrolysis to achieve dodecanethiol modified Rh(Rh@SC_(12)H_(2)5/CFC)for electrocatalytic nitrogen reduction reaction(NRR).The results demonstrate that after pyrolysis for 0.5 h at 150℃,the obtained Rh@SC_(12)H_(2)5/CFC-0.5 exhibits excellent NRR activity with an NH3 yield rate of 121.2±6.6μg∙h^(−1)∙cm^(−2)(or 137.7±7.5μg∙h^(−1)∙mgRh^(−1))and a faradaic efficiency(FE)of 51.6%±3.8%at−0.2 V(vs.RHE)in 0.1 M Na_(2)SO_(4).The theoretical calculations unveil that the adsorption of dodecanethiol on the hollow sites of Rh(111)plane is thermodynamically favorable,effectively regulating the electronic structure and surface wettability of metallic Rh.Importantly,the dodecanethiol modification on Rh(111)obviously decreases the surface H*coverage,thus inhibiting the competitive hydrogen evolution reaction and concurrently reducing the electrocatalytic NRR energy barrier.

Durability of Hepatitis B surface antigen seroclearance in patients experienced nucleoside analogs or interferon monotherapy: A real-world data from Electronic Health Record

Little is known about the difference in durability of HBsAg seroclearance induced by nucleoside analogs (NAs) or by interferon (IFN). A real-world, retrospective cohort study was conducted. Patients were assigned into two groups: NAs monotherapy-induced HBsAg seroclearance subjects and IFN monotherapy induced-HBsAg seroclearance subjects. A total of 198 subjects, comprised by 168 NAs monotherapy-induced and 30 IFN monotherapy-induced, who achieved HBsAg seroclearance were included in this study. The one-year probabilities of confirmed HBsAg seroclearance were significantly different in patients with NAs monotherapy and IFN monotherapy (0.960 (with 95% CI 0.922–0.999) vs. 0.691 (with 95% CI 0.523–0.913), log-rank-P = 4.04e-4). 73.3% (11 of 15) HBsAg recurrence occurred within one year after HBsAg seroclearance. The one-year probabilities of confirmed HBsAg seroclearance were higher in IFN monotherapy patients with anti-HBs than in IFN monotherapy patients without anti-HBs (0.839 (with 95% CI 0.657–1.000) vs. 0.489 (with 95% CI 0.251–0.953), log-rank test, P = 0.024). Our study thus provided novel insights into the durability of HBsAg seroclearance induced by NAs or IFN monotherapy. In particular, the HBsAg seroreversion rate was relatively high in IFN monotherapy subjects. The presence of anti-HBs was significantly correlated with a longer durability of functional cure induced by IFN treatment. And one-year follow-up in HBsAg seroclearance achieved individuals is proper for averting HBsAg seroreversion and other liver disease.