INTERNATIONAL IMMUNOPHARMACOLOGY
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2024
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IF 4.8
Shengsheng Mei,Shanshan Peng,Eu Gene Vong,Jinbiao Zhan
Background Clinical data indicate that a substantial portion of cancer patients, though eligible for immune checkpoint inhibitor (ICI) therapy, cannot fully benefit from ICI monotherapy due to the poor immunogenicity of tumors and lack of tumor-infiltrating lymphocytes within the ‘cold’ tumor microenvironment (TME). In addition to poor antibody penetrance into the TME, systemic delivery of ICIs is associated with immune-related adverse events (irAEs) among recipients, some of which are life-threatening. Oncolytic virotherapy is a potentially viable approach to improving the efficacy of ICI therapy because of their ability to selectively replicate and lyse tumor cells, release tumor-associated antigens (TAAs), induce inflammatory response and promote lymphocyte infiltration in tumors. Methods A recombinant oncolytic adenoviruses (OAd), denoted ZD55-aPD-L1 scFv, which carried the expression cassette for anti-PD-L1 scFv was constructed by molecular cloning. Western blot and ELISA assay were performed to detect aPD-L1 scFv expression. Flow cytometry were used to analyse PD-L1 expression and count tumor cells. Co-culture assay of human peripheral blood mononuclear cells (PBMCs) with tumor cells in vitro and triple-negative breast cancer (TNBC) MDA-MB-231 tumor-bearing model in vivo were evaluated the antitumor effects of recombinant oncolytic adenoviruses ZD55-aPD-L1 scFv. Results We found that cells infected with recombinant oncolytic adenovirus ZD55-aPD-L1 scFv can effectively express aPD-L1 scFv, which function similarly to its full-length anti-PD-L1 antibody. PBMCs have inherently very limited killing effect on tumor cells even with administration of anti-PD-L1 antibody as observed from our in vitro co-cultures. Treatment consisting of ZD55 alone or ZD55 combined with anti-PD-L1 antibody yielded mediocre antitumor efficacy in subsequent in vitro and in vivo investigations, but were all substantially surpassed by the synergistic antitumor effects observed with ZD55-aPD-L1 scFv treatment. We show that the concomitant direct oncolysis by the recombinant OAd and localized autocrine/paracrine interception of PD-1:PD-L1 checkpoint interaction mediated by ZD55-aPD-L1 scFv-infected cells is exceedingly superior to co-administration of ZD55 and anti-PD-L1 antibody in the human TNBC mice model. Conclusions Our results provided evidence for the development of novel strategies, in this case an anti-PD-L1 scFv-armed OAd, to bolster immune responses to ‘cold’ tumors and to improve therapeutic responsiveness to ICIs.
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高影响因子
BIOMATERIALS
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2024
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IF 12.8
Yue Xiong,Chao He,Junyang Qi,Meimei Xiong,Shuna Liu,Jingxin Zhao,Yuzhen Li,Gan Liu,Wenbin Deng
The tumor microenvironment in glioblastoma (GBM) is characterized by a pronounced immunosuppressive state, which significantly hampers tumor treatment and contributes to treatment resistance. While our previous research established that black phosphorus nanosheets (BPNS) inhibited glioblastoma cell migration and invasion, the impact of BPNS on the anti-tumor-associated immune mechanism remains unexplored. This study firstly investigated whether BPNS could modulate the tumor microenvironment through immunotherapy and elucidated the underlying mechanisms. We used a subcutaneous mouse model of GBM, which evaded immune surveillance to evaluate BPNS effects on immune cells within the tumor microenvironment. Our results demonstrated that BPNS significantly enhanced the tumor-suppressive microenvironment, reactivating immune cells' cytotoxicity against tumor cells. Moreover, further analysis revealed that BPNS counteracted the immunosuppressive state by reducing the expression of the immunosuppressive molecule PD-L1 in tumor cells, leading to an anti-tumor effect. Mechanistically, BPNS reduced PD-L1 expression through two main pathways: by inducing autophagy via binding to the HSP90 protein, leading to PD-L1 degradation through the autophagy pathway, and by inhibiting the PI3K-AKT signaling pathway, which reduced PD-L1 mRNA levels. This study expands the understanding of BPNS biological activity and suggests new strategies for utilizing BPNS as an adjuvant in immunotherapy.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yumo Li,Jikai Ye,Tian Xu,Guanglin Xia,Xuebin Yu
Dodecahydro-N-ethylcarbazole (12H-NEC) is considered as a highly promising liquid organic hydrogen carrier, but its commercial application is constrained by the requirement of large amounts of precious metal catalysts for dehydrogenation. Herein, Pd nanoclusters with an average particle size of 1.1 nm supported on amine groups modified carbon blacks (Pd/N–C HNO3 ) are developed to efficiently catalyze the dehydrogenation of 12H-NEC with a low loading of Pd (2.2 wt%, 0.12 mol%). Induced by the nitrogen doping in the carbon black, the d- band center of the Pd (111) surface shifts from −1.64 eV to −1.53 eV, resulting in the electron-deficient structure of thus-formed Pd nanoclusters owing to the electron transfer from Pd to N atoms and uniform distribution of Pd nanoclusters inside of carbon blacks. This electron transfer effectively tunes Pd 0 :Pd δ+ ratio for enhancing the adsorption of reactant species of 12H-NEC on the surface of Pd nanoclusters and hence facilitates the catalytic role of Pd nanoclusters in enhancing the hydrogen desorption performance of 12H-NEC. As a result, every step of the dehydrogenation of 12H-NEC under the catalysis of Pd nanoclusters on the nitrogen-doped support exhibits lower ΔG values compared to the non-doped support, which provides direct evidence to the important role of the nitrogen doping of the catalyst support in improving the dehydrogenation performance of 12H-NEC on the Pd surface. Therefore, a hydrogen release capacity of 5.60 wt% with 100% conversion and a selectivity of 90% could be obtained for 12H-NEC under the catalysis of Pd nanoclusters supported on amine-functionalized carbon black at 453 K with a low precious metal dosage (0.12 mol%).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2012
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IF 3.07
Changliang Huang,Hongye Zhang,Yanfei Zhao,Sha Chen,Zhimin Liu
Diatomite supported Pd–M (M = Cu, Co, Ni) bimetal nanocatalysts with various metal compositions were prepared and characterized by means of X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy. It was demonstrated that the metal nanoparticles were uniformly distributed on the support, and their size was centered around 8 nm with a relatively narrow size distribution. The catalysts were used to catalyze hydrogenation of long-chain aliphatic esters, including methyl palmitate, methyl stearate, and methyl laurate. It was indicated that the all diatomite-supported Pd-based bimetal catalysts were active to the selective hydrogenation of long-chain esters to corresponding alcohols at 270 °C, originated from the synergistic effect between the metal particles and the diatomite support. For the selective hydrogenation of methyl palmitate, Pd–Cu/diatomite with metal loading of 1% and Pd/Cu = 3 displayed the highest performance, giving a 1-hexadecanol yield of 82.9% at the substrate conversion of 98.8%.
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2012
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IF 2.947
Shaozhong Li,Wei Zhang,Man-Ho So,Chi-Ming Che,Runming Wang,Rong Chen
A facile solvothermal synthetic route has been successfully developed to fabricate Pd/Fe 3 O 4 nanocomposite with the assistance of polyvinylpyrrolidone (PVP) in N,N-dimethylformamide (DMF) solution. The as-prepared Pd/Fe 3 O 4 nanocomposite was composed of uniform 5 nm-sized Pd nanoparticles and Fe 3 O 4 nanocrystals with dimension of 40 nm. In this fabrication, PVP played an important role as a capping agent. The as-prepared Pd/Fe 3 O 4 nanocomposite exhibited superior catalytic performance and stability for various Suzuki coupling reactions, compared with single-component Pd nanoparticles under the same reaction conditions. More importantly, it displayed good magnetic property and could be easily separated from the reaction mixture by using a magnet and recycled for 10 times without losing its catalytic activity.
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JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Lina Guo,Ligang Yan,Ruijun Xie,Limin Han,Ning Zhu
In this work, we investigate a palladium complex exhibiting aggregation-induced emission enhancement (AIEE) properties and remarkable solvatochromism behavior driven by structural changes arising from solvent-solute interactions. Specifically, in polar aprotic solvents, the color of the Pd complex changes from blue to purple as solvent polarity increases, accompanied by a blue shift in the UV–Vis spectrum. Notably, this blue shift is even more pronounced in polar protic solvents, which also show a significant increase in fluorescence emission. These effects are likely driven by hydrogen-bond interaction between the protic solvents and the Pd complex. Density Functional Theory (DFT) calculations show that increased solvent polarity significantly alters the electronic distribution of the Pd complex. Higher solvent polarity leads to a higher orbital transition energy, resulting in a blue shift in the UV–Vis absorption spectrum. X-ray single-crystal structure analysis further reveals that hydrogen-bonding interactions between the Pd complex and methanol stabilize its planar structure. When water is introduced, the Pd complex undergoes aggregation through non-covalent interactions, which modify the stacking arrangement. This change weakens the π-π interactions between adjacent molecules, thereby minimizing energy loss in the system. Consequently, the Pd complex effectively utilizes the AIEE mechanism to detect water content in methanol.
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Molecular Catalysis
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2024
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IF 3.9
Xing Gao,Wenna Zhang,Yingying Ruan,Shihao Zhang,Sheng Wei,Yiwen Zhang,Pengfei Liu,Dong Tian,Yihu Dai,Yanhui Yang
The conversion of biomass-based compounds into highly value-added chemicals has received extensive attention in recent years. This work reports the liquid-phase selective hydrogenation and furan ring-rearrangement of furfural (FFL) into cyclopentanone (CPO) and cyclopentanol (CPL) over Pd/Co 4 Al 1 -HTs catalysts and water as the solvent. The specific reaction rate of the optimal catalyst at 160 °C reaches 538 h –1 , and the selectivity of CPO/CPL is 77.5 %. By adopting the ion-exchange and formamide treatment methods, the type of the interlayer anions and interlayer spacing for the CoAl-HTs supports can be regulated, which can affect the state of the supported Pd sites and their catalytic activity and selectivity towards the ring-rearrangement products. Furthermore, the H 2 /D 2 exchange experimental results demonstrate that the presence of the interlayer NO 3 – anions of CoAl-HTs support promotes the activation and dissociation of H 2 , thereby accelerating the hydrogenation of FFL to cyclic compounds.
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SOLID STATE SCIENCES
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2024
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IF 3.4
Dong Yanping,Xiqiang Tian,Hongji Zhao,Jintao Luo
The fabrication of small Pd nanoparticles (NPs) anchored on titanium dioxide (TiO 2 ) supports remains a great challenge due to its high surface energy. Herein, flower-like three dimensional (3D) TiO 2 microstructures assembled from needle flakes are fabricated thru a facile evaporation-induced assisted hydrothermal method, and then modified with amines group (3D-TiO 2 -NH 2 ). Small and uniform dispersed Pd nanoparticles were anchored on the surface of 3D-TiO 2 -NH 2 supports using polyol reduction method. Remarkably, the obtained 3D-TiO 2 -NH 2 supported Pd-based catalyst (Pd@3D-TiO 2 -NH 2 ) demonstrated an optimal 4-NP catalytic hydrogenation efficiency ( k = 1.09 min −1 ), which is 1.56 and 3.52 times superior than that of the Pd@3D-TiO 2 ( k = 0.699 min −1 ) and Pd@TiO 2 –P25 ( k = 0.31 min −1 ) catalysts, respectively. In-depth investigation of the structure-property relationship by SEM, XRD, N 2 adsorption-desorption isotherm, TEM, XPS, CO chemisorption and CO-FTIR reveal that the optimal catalytic hydrogenation activity of Pd@3D-TiO 2 -NH 2 can be credited to its 3D hierarchical structure (interconnected needle flakes) and the amines group existing on the surface of flower-like three dimensional hierarchical TiO 2 , which control the Pd particles size (2.7 nm) and uniform dispersion (43.5%) to generate more surface active Pd 0 entities over Pd@3D-TiO 2 -NH 2 .
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JOURNAL OF CONTROLLED RELEASE
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2024
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IF 10.5
Xiaoxuan Wang,Fangxuan Li,Jialu Zhang,Lu Guo,Mengmeng Shang,Xiao Sun,Shan Xiao,Dandan Shi,Dong Meng,Yading Zhao,Chao Jiang,Jie Li
PD-1/PD-L1-based immune checkpoint blockade therapy has shown limited benefits in tumor patients, partially attributed to the inadequate infiltration of immune effector cells within tumors. Here, we established a nanoplatform named DPPA/IL-15 NPs to target PD-L1 for the tumor delivery of IL-15 messenger RNA (mRNA). DPPA/IL-15 NPs were endowed with ultrasound responsiveness and contrast-enhanced ultrasound (CEUS) imaging performance. They effectively protected IL-15 mRNA from degradation and specifically transfected it into tumor cells through the utilization of ultrasound-targeted microbubble destruction (UTMD). This resulted in the activation of IL-15-related immune effector cells while blocking the PD-1/PD-L1 pathway. In addition, UTMD could generate reactive oxygen species (ROS) that induce endoplasmic reticulum (ER) stress-driven immunogenic cell death (ICD), initiating anti-tumor immunity. In vitro and in vivo studies revealed that this combination therapy could induce a robust systemic immune response and enhance anti-tumor efficacy. Thus, this combination therapy has the potential for clinical translation through enhanced immunotherapy and provides real-time ultrasound imaging guidance.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yang Li,Jingjing Yu,Jianshan Zeng,Yinyue Ye,Qiao Yin,Yingshan Zeng,Zhi Liu
The utilization of CO 2 photoreduction into valuable hydrocarbon fuels presents a promising avenue for mitigating climate change and providing a sustainable energy source. However, photogenerated carriers are highly prone to recombination, which adversely affects photocatalytic activity. In our study, we introduce a novel photocatalyst synthesis method, featuring an Ohmic contact (OC) structure that incorporates biomass-derived hollow carbon microspheres (HCM), Pd nanocubes (NC), and Indium Oxide (In 2 O 3 ) through a simple yet effective thermal reduction method. This modification significantly enhances the photocatalytic efficiency of the Pd NC/In 2 O 3 /HCM (donated as PIC) system, achieving an optimal value of 496.89 μmol∙g −1 over 5 h without the need for additional additives, 8.7-fold higher than that of the pristine In 2 O 3 . Experimental and theoretical results reveal that the substantial enhancement in CO 2 photoreduction performance can be attributed to the ultra-low resistance (122 Ω) interfaces within the PIC system, facilitating accelerated transfer of photogenerated electrons. This work provides a strategy for boosting CO 2 photoreduction efficiency by the reduction of interface resistance to promote rapid photogenerated electron migration.
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APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Jie Liu,Youlin Xiong,Ting Wu,Xining Zhang,Jialin Zhao,Shuangfei Cai,Wei Zhang,Rong Yang
Rational design and controllable construction of supported nanostructures with excellent antibacterial property remain a great challenge. Recently, transition metal carbides/nitrides/carbonitrides (MXenes) have attracted much interest in many fields due to their large specific surface areas and good photothermal property. Herein, a simple yet effective surface engineering strategy based on the tuning of MXene surface chemistry is presented, which allows in-situ controlled growth of the Pd nanocubes on the V 2 CT x nanosheets. Briefly, the exfoliated V 2 CT x nanosheets by HF are annealed, which changes the composition of surface terminations while creating the mesoporous structures. The annealing largely affects the exposure and oxidation states of the adjacent V atoms and allows the controllable growth of Pd nanocubes. Interestingly, the obtained Pd@V 2 CT x nanocomposites show enhanced peroxidase-/oxidase-like activities and intrinsic photothermal effect in the near infra-red (NIR) region due to the strong metal-support interaction. Furthermore, the combined nanocatalytic-photothermal treatment by their versatilities remarkably improves the antibacterial efficacy, giving a high killing rate (above 98 % for both Escherichia coli and Staphylococcus aureus ). This work provides a new avenue to develop the supported metal nanostructures based on MXenes for antibacterial application.
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JOURNAL OF MATERIALS SCIENCE
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2024
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IF 3.5
Chu Siyu,Sun Min,Kang Liping,Guo Xiaowen,Wang Haiyan,Li Bin,Li Zijiong
Although carbon-based catalysts show great potential in oxygen reduction reaction (ORR), it is still a challenge to increase their catalytic efficacy while reducing the amount of precious metals such as platinum and palladium. In this research, a palladium–silver bimetallic catalyst (Pd–Ag/CD) was flexibly synthesized through the in-situ self-reduction of palladium chloride and silver nitrate by carbon dots (CD). This novel catalyst displayed remarkable activity for the ORR, with peak potential, onset potential, and half-wave potential recorded at 0.89 V, 1.004 V, and 0.88 V, respectively. The exceptional performance of Pd–Ag/CD is attributed to the synergistic adjustment of the d-band by the palladium and silver metals, which optimizes the adsorption of oxygen and boosts the reaction's overall activity. Additionally, the slight negative shift of 12 mV in the half-wave potential after 5000 cycles indicates the catalyst's excellent durability. The findings of this study offer valuable theoretical insights for the development of carbon nanomaterial-based catalytic systems.
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