JOURNAL OF NANOBIOTECHNOLOGY
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2024
·Vol. 22
·期 1
·1-20
·
IF 10.6
Guo Hong,Li Xia,Mao Dengxuan,Wang Hong,Wei Liangyin,Qu Ding,Qin Xiaoying,Li Xiaoqi,Liu Yuping,Chen Yan
The insufficient abundance and weak activity of tumour-infiltrating lymphocytes (TILs) are two important reasons for the poor efficacy of PD-1 inhibitors in hepatocellular carcinoma (HCC) treatment. The combined administration of tanshinone II A (TSA) and astragaloside IV (As) can up-regulate the abundance and activity of TILs by normalising tumour blood vessels and reducing the levels of immunosuppressive factors respectively. For enhancing the efficacy of PD-1 antibody, a magnetic metal–organic framework (MOF) with a homologous tumour cell membrane (Hm) coating (Hm@TSA/As-MOF) is established to co-deliver TSA&As into the HCC microenvironment. Hm@TSA/As-MOF is a spherical nanoparticle and has a high total drug-loading capacity of 16.13 wt%. The Hm coating and magnetic responsiveness of Hm@TSA/As-MOF provide a homologous-magnetic dual-targeting, which enable Hm@TSA/As-MOF to counteract the interference posed by ascites tumour cells and enhance the precision of targeting solid tumours. Hm coating also enable Hm@TSA/As-MOF to evade immune clearance by macrophages. The release of TSA&As from Hm@TSA/As-MOF can be accelerated by HCC microenvironment, thereby up-regulating the abundance and activity of TILs to synergistic PD-1 antibody against HCC. This study presents a nanoplatform to improve the efficacy of PD-1 inhibitors in HCC, providing a novel approach for anti-tumour immunotherapy in clinical practice.
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高影响因子
FUEL
·
2024
·
IF 6.7
Huan Zhang,Junhong Li,Xinyu Huang,Xuemin Duan,Ruirui Yue,Jingkun Xu
Design and preparation of catalysts with lower cost and higher catalytic efficiency are still important strategy to promote the wide application of alkaline direct alcohol fuel cells (ADAFCs). In this study, a novel anode catalyst for ADAFCs has been easily synthesized based on polyaniline (PANI)-modified wrinkled reduced graphene oxide (rGO) and Pd nanoparticles (Pd NPs). Morphology and structure characterization confirm the modified lamellar structure and composition of the Pd/PANI-rGO composite, and X-ray photoelectron spectroscopy (XPS) demonstrates the electron transfer from PANI-rGO to Pd NPs. For ethylene glycol and ethanol oxidation reactions (EGOR/EOR) in alkaline media, the Pd/PANI-rGO exhibits promising electrocatalytic properties with mass activity as 4342.5 and 2220.4 mA mg Pd -1 , specific activity as 26.6 and 13.6 mA cm - 2 and intrinsic activity as 5.7 and 2.5 s - 1 , respectively. Moreover, the Pd/PANI-rGO shows significantly enhanced anti-poisoning ability and durability as compared with contrast samples due to the well dispersion of Pd NPs on PANI-rGO and the synergistic interaction between PANI-rGO and Pd NPs producing electron-rich Pd and more active sites for EGOR and EOR. This work is expected to provide theoretical foundation for designing low-cost and high-efficiency ADAFCs anode catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Lina Xiao,Qiuping Zhang,Xinzhi Wang,Bowen Li,Xiaoyan Li,Xiaojian Yang,Wenxuan Li,Hao Zhang
A significant enhancement in the photocatalytic activity of metal–organic framework (MOF) is achieved by expanding the visible-light response range through the strategic incorporation of functional groups, such as metalloporphyrins. Herein, Pd-metalised tetrakis(4-carboxyphenyl)porphyrin (PdTCPP) photosensitiser is integrated into the UiO-66-(NH 2 ) 2 framework, creating the hybrid material PdTCPP ⊂ UiO-66-(NH 2 ) 2 using a facile mixed-ligand strategy. Platinum nanoparticles (Pt NPs) are subsequently introduced as a co-catalyst via in situ photoreduction, resulting in the formation of the Pt/PdTCPP ⊂ UiO-66-(NH 2 ) 2 hybrid material, which demonstrates exceptional catalytic performance under visible-light irradiation. Specifically, the photocatalytic hydrogen production rate for 1 % Pt/PdTCPP ⊂ UiO-66-(NH 2 ) 2 reaches 1152 μmol g −1 h −1 . The quantum yield (QY) and space–time yield (STY) of 1 % Pt/PdTCPP ⊂ UiO-66-(NH 2 ) 2 at 400 nm radiation are approximately 1.21 % and 0.24 %, respectively. This excellent hydrogen production performance is attributed to the rapid transfer of long-lived electrons generated by the photoexcitation of Pd-porphyrin photosensitiser to Pt NPs, improving the separation efficiency of photogenerated electrons and holes. These findings demonstrate the combining photosensitisers potential with co-catalysts in MOFs, developing highly efficient photocatalysts for hydrogen production, which offers a promising avenue for the development of sustainable energy materials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xiaofeng Liu,Xudong Chen,Chunying Wang,Shaohua Xie,Jingyi Wang,Yaobin Li,Fudong Liu,Hong He
Usually, active hydroxyl groups play a crucial role in the catalytic oxidation of formaldehyde (HCHO), especially on supported noble metal catalyst systems. However, in present work, we observed an unexpected phenomenon where H 2 O exhibited an inhibitory effect on Pd/SiO 2 catalyst for HCHO oxidation. The activity of Pd/SiO 2 catalyst could be significantly improved by constructing Si and O double vacancy-defects (V Si V o , through acid-base etching) and oxygen vacancy defects (V o , through H 2 reduction). Interestingly, the inhibiting effect of H 2 O on HCHO oxidation was completely reversed to a promotion effect on the Pd/SiO 2 -(V Si V o ) catalyst, which was due to the fact that such catalyst had the ability to continuously activate H 2 O producing reactive hydroxyl species. Reaction mechanism study revealed that the HCHO oxidation on all Pd/SiO 2 catalysts followed two reaction pathways: (1) HCHO → HCOO → CO 2 ; (2) HCHO → CHO → CO → CO 2 , while the difference of active hydroxyl content on the catalysts resulted in varying degrees of formate accumulation on the catalyst surfaces. This study provides a promising strategy to enhance the H 2 O resistance of Pd catalysts and design high-performance noble metal catalysts for catalytic HCHO oxidation.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
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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SOLID STATE SCIENCES
·
2024
·
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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BIOMATERIALS
·
2024
·
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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Biomaterials Science
·
2020
·Vol. 8
·期 17
·4757-4766
·
IF 6.183
Jing Zhang,Dan Liu,Jiale Liu,Yanfeng Han,Haiyan Xu,Xigang Leng,Deling Kong,Lanxia Liu
Combined blockades of CTLA-4 and PD-1 can yield better overall complementary clinical outcomes than individual blockades, but the response rates are still relatively low. To investigate the anti-tumor effects of various combined strategies, we designed various spherical nucleotide nanoparticles (SNPs) loaded with CTLA-4 aptamer (cSNPs), PD-1 siRNA (pSNPs) or both (hybrid SNPs, or hSNPs). The results demonstrated that hSNPs could promote significantly stronger anti-tumor immune responses in a nonredundant fashion than the mixture of pSNPs and cSNPs (pSNPs & cSNPs). We reasoned that this is because all individual immune cells could receive both CTLA-4 and PD-1 blockades when they engulfed hSNPs, but it is much less likely that individual immune cells could receive both CTLA-4 and PD-1 blockades as many of them may not take both pSNPs and cSNPS from pSNPs & cSNPs. Further results revealed that the synergistic immune stimulatory effects of CTLA-4 and PD-1 blockades in the form of hSNPs were at least partly through regulating the immune suppressive function of both Tregs and TIM3+ exhausted-like CD8 T cells and allowing effector T cells to expand. This mechanism is not identical to earlier reported mechanisms of CTLA-4 and PD-1 blockades.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
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
·
2024
·
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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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yunhua Li,Shiyu Zheng,Yuting He,Shui Yang,Wei-Hsiang Huang,Chih-Wen Pao,Zhiwei Hu,Xiaoqing Huang
The coordination environments of isolated metals significantly influence the catalytic properties of materials. However, challenges persist in the precise modulation of these microenvironments. In this study, we achieved atomically dispersed Pd on sulfur-doped tin dioxide (SnO 2 ) through the controlled oxidation of SnS 2 nanosheets pre-loaded with single-atom Pd (Pd/SnS 2 ). Our findings reveal that the synthesized catalyst features a central single-atom Pd, which coordinates with oxygen and tin in the first coordination shell and sulfur binding tin in the second shell. The coordination of isolated Pd with sulfur in the out-of-plane second shell layer enhances oxygen adsorption while inhibiting O O dissociation, thus directing hydrogen peroxide selectivity. This results in a higher productivity and durability of hydrogen peroxide compared to pristine Pd/SnS 2 and traditional samples. This work presents an effective strategy to tailor and preserves the coordination micro-environment of central single-atom metals during catalytic reactions.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2024
·Vol. 99
·期 4
·978-988
·
IF 2.8
Likai Dai,Zheng Fang,Anxian Peng,Yunhong Chen,Yitong Liu,Huimei Chen,Rongjun Yan,Rencheng Zhou,Mingming Du
BACKGROUND Photothermal catalytic oxidation technology for synthesis of high value-added chemicals has become a hot topic of research at home and abroad. As a special structure, titania (TiO 2 ) nanotubes (Ti-NTs) possess larger specific surface area and adsorption capacity, which have shown great application prospects in photothermal catalytic oxidation. RESULTS In this work, high-performance palladium (Pd-Ti-NTs catalyst were prepared and applied to the photothermal catalytic oxidation of 5-hydroxymethyl (HMF) and benzyl alcohol. The photothermal dependence on catalytic activity and selectivity of HMF and benzyl alcohol oxidation was studied in detail. The results revealed that compared with thermal catalytic oxidation, the catalysts showed significantly higher conversions of both benzyl alcohol and HMF under light. in particular, HMF conversion increase from 55.6% to 99.7%. Aldehyde oxidation is inhibited by alcohol and can be dramatically promoted by light radiation. This is probably because alcohol can inhibit the adsorption of aldehyde, and this inhibiting effect is weakened through light radiation, thus promoting the oxidation of aldehydes. Therefore, the selectivity of the final products 2,5-furandicarboxylic acid (FDCA) and benzoic acid were dramatically increased in both systems under light radiation, and the selectivity for FDCA was obviously increased from 5.8% to 61.3%, and the yield reached 61.0%, which is higher than that of most of the reported Pd-TiO 2 -based catalysts for FDCA. CONCLUSIONS In this paper, we verify that Pd-Ti-NTs could preferentially promote the conversion of aldehydes to acids in the presence of light, and obtained catalysts with high catalytic performance and high stability for benzyl alcohol and HMF oxidation. © 2024 Society of Chemical Industry (SCI).
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