CHEMISTRY-A EUROPEAN JOURNAL
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2022
·Vol. 29
·期 16
·e202203142
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IF 5.02
Jingwen Luo,Anqi Huang,Yao-Yue Yang,Xing-Yu Ma,Quan-Liang Chen,Junxian Chen,Yajuan Wu
Graphical Put to good use : A Pd-doped Co (Pd/Co) catalyst with high Pd atom utilization efficiency was designed and prepared for hydrogenation of nitroarenes. Its catalytic activity was much better than commercial Pd powder (>150 times) in nitrobenzene hydrogenation reaction. This work might provide a simple and low-cost methodology to design and synthesize highly efficient catalysts. Enhancing catalytic performance as well as reducing catalyst cost are the eternal pursuit for the catalysis community. Herein, a simple and effective palladium-doped cobalt (Pd / Co) catalyst with high Pd atom utilization efficiency was synthesized via galvanic replacement reaction for the selective hydrogenation of nitrobenzene with H 2 at room temperature, delivering >99 % yield of aniline with up to 158 times higher catalytic activity than commercial palladium powder. Detailed characterizations and DFT calculations revealed that Co−Pd interaction leads to a decrease in electron density of Pd and the distance between Pd atoms that results in the enhanced catalytic performance. Further experiments indicated that the Pd / Co catalyst serves as a highly efficient, selective, and recyclable catalyst for a range of nitroarene substrates. This work might provide a green and sustainable methodology to design and synthesize highly active catalysts with high utilization efficiency of the noble metals in fundamental and applied research.
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Advanced Science
·
2024
·
IF 14.3
Tianliang Li,Dan Xu,Zhao Ruan,Jie Zhou,Wenbo Sun,Bo Rao,Haibo Xu
Intrinsic immunosuppressive tumor microenvironment (ITM) and insufficient tumor infiltration of T cells severely impede the progress of glioblastoma (GBM) immunotherapy. In this study, it is identify that inhibiting the expression of glucose transporter 1 (GLUT1) can facilitate the prevention of lactate excretion from tumor glycolysis, which significantly alleviates the lactate-driven ITM by reducing immunosuppressive tumor-associated macrophages (TAMs) and regulatory T cells (Tregs). Simultaneously, the findings show that the generated inflammatory cytokine IFN-γ during immune activation aggravates the immune escape by upregulating immune checkpoint programmed death-ligand 1 (PD-L1) in tumor cells and TAMs. Therefore, an injectable thermogel loaded with a GLUT1 inhibitor BAY-876 and a PD-1/PD-L1 blocker BMS-1 (Gel@B-B) for dual-regulation of metabolism and immunity of GBM is developed. Consequently, in situ injection of Gel@B-B significantly delays tumor growth and prolongs the survival of the orthotopic GBM mouse model. By actively exposing tumor antigens to antigen-presenting cells, the GBM vaccine combined with Gel@B-B is found to significantly increase the fraction of effector T cells (Th1/CTLs) in the tumor microenvironment, thereby remarkably mitigating tumor recurrence long-term. This study may provide a promising strategy for GBM immunotherapy.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhongming Wang,Hang Yuan,Siting Chen,Yong Jia,Lina Guo,Hong Wang,Wenxin Dai
The progressive transfer of photogenerated electrons between the catalyst components and reactants is of great significance for photocatalysis. Amorphous Pd (Pd A ) and oxygen vacancies (V O s) were simultaneously introduced in Pd-In 2 O 3 exploiting hydrogen-induced amorphization effects; 0.6 wt% Pd-In 2 O 3 exhibited a 4.5-fold increase in activity and a 3.2-fold higher selectivity toward CH 3 OH + CO (63.62 %) compared with In 2 O 3 . Multiple in situ techniques and theoretical calculations revealed that intercomponent electron transfer channels were established via various interface structures formed between Pd A or crystalline Pd (Pd C ) and In 2 O 3 ; Pd A acted as electronic pump, facilitating the transfer and separation of photogenerated electrons, resulting in their subsequent enrichment on the surface of Pd A . Simultaneously, Pd A acted as electron-donating adsorption site for H 2 O, increasing the number of electrons received by H 2 O, further inhibiting the competitive adsorption of H 2 O and CO 2 on V O sites, and promoting the hydrogen evolution reaction. Additionally, the electronic coupling between Pd C and V O s could significantly decrease the electron-donating ability of V O s, reducing the number of electrons received by CO 2 , thus effectively regulating the degree of CO 2 reduction. This study employs Pd A /Pd C and V O s to synergistic optimize the progressive transfer of photogenerated electrons, and presents a novel approach for elucidating the catalytic mechanism.
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Chemistry-An Asian Journal
·
2019
·Vol. 14
·期 19
·3397-3403
·
IF 3.698
Chunjie Li,Hongjie Yu,Songliang Liu,You Xu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Graphical Being rattled : Pt-based nanorattle-structured materials consisting of Pd core and mesoporous PtRu shell (Pd@mPtRu NRs) have been prepared by a facile method. Benefitting from the superior morphology and composition, the obtained Pd@mPtRu NRs could be used as efficient electrocatalyst for oxygen reduction reaction. Pt-based nanomaterials play important roles in the catalytic process toward oxygen reduction reaction (ORR). Rationally regulating the composition and morphology of the catalysts could enhance the catalytic performance effectively. In this work, an effective method is presented to synthesize Pd@ mesoporous PtRu nanorattles (Pd@mPtRu NRs) containing a Pd core and a mesoporous PtRu shell. Owing to the unique structure and PtRu alloy composition, the prepared Pd@mPtRu NRs exhibit an enhanced catalytic performance and durability toward ORR relative to mesoporous PtRu hollow nanoparticles (mPtRu HNs) and commercial Pt/C. The proposed approach may provide a general way to synthesize Pt-based yolk-shell structures with different compositions.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 72
·18187-18192
·
IF 5.317
Jishi Chen,Liren Liu,Xu Liu,Lingwen Liao,Shengli Zhuang,Shiming Zhou,Jinlong Yang,Zhikun Wu
Graphical Double-crown Pd 4 (PET) 8 and Pd 5 (PET) 10 were successfully doped with gold through two Au atoms replacing one Pd atom with the other double-crown structure essentially unchanged. Au 4 Pd 2 (PET) 8 is the smallest chiral bimetal nanoclusters so far and it bears chirality originating from not only the helixed Au 4 Pd 2 S 8 framework but also unanimous R or S configuration of sulfur atoms in the enantiomer. Double-crown Ni, Pd, or Pt nanoclusters have attracted extensive interests due to their aesthetic structure and intriguing properties. However, their doping by other metals remains unknown until now. Herein, Pd 4 (PET) 8 and Pd 5 (PET) 10 (PET: SCH 2 CH 2 Ph) were successfully doped with gold and the doped nanoclusters were characterized by using multiple techniques such as mass spectrometry and X-ray crystallography. It is revealed that in the doping not one but two gold atoms replace one Pd with the other double-crown structure essentially unchanged, and the gold-doping results in the blue-shift of the maximum visible absorption, the increase of optical energy gap and the reduction of anti-aromaticity of monometal Pd nanoclusters. Importantly, it is found that Au 4 Pd 2 (PET) 8 nanocluster bears chirality originating from not only the helixed Au 4 Pd 2 S 8 framework, but also unanimous R or S configuration of sulfur atoms in the enantiomer. For the latter chirality origin, it was not previously reported or proposed. Au 4 Pd 2 (PET) 8 reported here also represents the smallest chiral bimetal nanocluster so far to the best of our knowledge. This work advances one step toward both the tailoring of group 10 metal nanoclusters by doping and the understanding of chirality origin for metal nanoclusters.
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Journal of Pharmaceutical Analysis
·
2025
·
IF 8.9
Weiming You,Zhengjun Zhou,Zhanfeng Li,Jin Yan,Yang Wang
Reprogramming oncogenic signaling pathways to generate anti-tumor effects is a promising strategy for targeted cancer intervention, without significant off-target effects. Although reprogramming multi-oncoprotein interactions in a single signaling pathway axis has been shown to achieve sustained efficacy, there are several challenges that limit its clinical application. Herein, we transformed the mouse double minute 2 homolog (MDM2)-heat shock cognate protein 70 (HSC70) axis, a tumor-promoting pathway, into an activator of anti-tumor immunity using the Path-editor, an artificial selenoprotein. Once it enters the cell, Path-editor decomposes into PMI and PPI peptides: PMI inhibits MDM2-mediated p53 degradation and promotes HSC70 expression, while PPI binds to HSC70, enabling its ability to selectively degrade the programmed cell death ligand 1 (PD-L1). As a proof of concept, we tested its performance in microsatellite-stable (MSS) colorectal cancer, which typically displays limited responsiveness to immunotherapy. The results indicated that Path-editor effectively attenuated PD-L1 expression and reversed immune evasion in both CT26 allografts and humanized patient-derived tumor xenograft (PDX) models, thereby inhibiting tumor progression with high biosafety. Therefore, this paper introduces Path-editor as a paradigm for reprogramming oncogenic multi-protein pathways, utilizing selenium-assisted approach to achieve the rapid design of tumor-specific pathway editors. This strategy is expected to reverse immune escape in MSS colorectal cancer and treat difficult malignancies.
研究领域:
肿瘤学
·
免疫学
·
分子生物学
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Materials Chemistry Frontiers
·
2020
·Vol. 4
·期 6
·1671-1678
·
IF 6.788
Ping She,Jun-sheng Qin,Heng Rao,Buyuan Guan,Jihong Yu
Efficient charge separation and light harvesting of photocatalysts (e.g., TiO2) are the key issues to be considered in the design of solar-energy conversion systems. In particular, the charge separation of noble metal-decorated TiO2 materials could be greatly improved via decreasing the size of noble metal particles (NPs). Furthermore, designing specific morphologies such as hollow structures can improve light harvesting ability. Herein, a hybrid hollow TiO2 with spatially separated bimetals (Pd@TiO2@Au) was prepared, which demonstrated enhanced charge separation. By choosing zeolite as the sacrificial substrate, ultrasmall Pd NPs and Au NPs were decorated in the inner and outer shells of hollow TiO2, respectively. The separated bimetals could pull the photoexcited electrons away from the surface of TiO2 for more efficient charge separation. The as-prepared Pd@TiO2@Au catalyst exhibited a superior photocatalytic H2 evolution rate up to 272.3 μmol h−1, which was higher than most of the TiO2-based photocatalysts.
研究领域:
材料科学
·
光催化
·
太阳能转换
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JOURNAL OF NANOBIOTECHNOLOGY
·
2025
·Vol. 23
·期 1
·1-20
·
IF 12.6
Cai Hai,Xue Panpan,Liu Siyuan,Ma Yaxin,Zeng Xuemei,Yan Shuangqian,Xu Ning
Elevated squalene epoxidase (SQLE) levels in bladder cancer cells drive abnormal cholesterol accumulation, contributing to malignancy, invasion, and resistance to immunotherapy. Here, we introduce a hollow CuO nanoparticle-based nanotherapeutic, termed CuOTeDsP, which is PEGylated and co-loaded with SQLE inhibitor terbinafine and disulfiram, for enhanced bladder cancer therapy through cholesterol metabolism modulation. CuO nanoparticles exhibit peroxidase-, catalase-, and glutathione oxidase-like enzymatic activities, along with biodegradability, resulting in elevated oxidative stress, alleviation of hypoxia, and responsive therapeutic release. Terbinafine reduces cholesterol levels in cancer cells by inhibiting SQLE, downregulating the expression of ATP7A and PD-L1, thereby promoting cellular Cu 2+ accumulation and enhancing immune responses. Disulfiram further reacts with Cu 2+ to form lethal bis(diethyldithiocarbamate)-copper complexes. Mechanistic studies reveal that CuOTeDsP induces cell death through a combination of cuproptosis and apoptosis, while simultaneously eliciting robust immune responses. In synergy with PD-1 monoclonal antibody, CuOTeDsP achieves a high tumor inhibition rate of 70% in a mouse bladder cancer model. This work highlights an effective strategy for bladder cancer by leveraging cuproptosis-driven immunotherapy and provides insights into the design of advanced nanotherapeutics.
Section
Graphical abstract
研究领域:
纳米医学
·
癌症生物学
·
免疫学
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代谢疾病
·
药学
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Catalysis Science & Technology
·
2015
·Vol. 6
·期 9
·3027-3037
·
IF 5.426
Yanan Liu,Yufei He,Daran Zhou,Junting Feng,Dianqing Li
Aiming at the preparation of catalysts with well-controlled structures, bimetallic PdCu catalysts containing only small amounts of Pd were prepared by two different methods for partial hydrogenation of acetylene. The highly dispersed and stable PdCu catalyst with the Pd : Cu atomic ratio of 1 : 40 was obtained from a Pd(OH)2/CuMgAl hydrotalcite (HT) precursor by a modified co-precipitation method. The obtained PdCu catalyst possessed uniform PdCu nanoalloys with an average size of 1.8 ± 0.3 nm. As a comparison, the impregnation method was also employed to prepare bimetallic PdCu catalysts and it was confirmed that the Pd-rich(core)–Cu-rich(shell) structure was dominant. Under identical reaction conditions, approximately 100% conversion and 82% selectivity at 100 °C were achieved using the PdCu nanoalloy catalyst which were 23% and 12% higher than those of the Pd-rich(core)–Cu-rich(shell) catalyst. The preferable activity was ascribed to the homogeneous nanoalloy structure and small size effect. The enhanced selectivity was attributed to the strong synergistic effect of PdCu. More significantly, this superior catalytic performance can be retained after 48 h of continuous reaction due to the excellent resistibility against carbon deposition and the confinement effect.
研究领域:
催化化学
·
材料科学
·
有机合成
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Journal of the American Chemical Society
·
2013
·
IF 10.677
An-Liang Wang,Han Xu,Jin-Xian Feng,Liang-Xin Ding,Ye-Xiang Tong,Gao-Ren Li
Low cost, high activity, and long-term durability are the main requirements for commercializing fuel cell electrocatalysts. Despite tremendous efforts, developing non-Pt anode electrocatalysts with high activity and long-term durability at low cost remains a significant technical challenge. Here we report a new type of hybrid Pd/PANI/Pd sandwich-structured nanotube array (SNTA) to exploit shape effects and synergistic effects of Pd-PANI composites for the oxidation of small organic molecules for direct alcohol fuel cells. These synthesized Pd/PANI/Pd SNTAs exhibit significantly improved electrocatalytic activity and durability compared with Pd NTAs and commercial Pd/C catalysts. The unique SNTAs provide fast transport and short diffusion paths for electroactive species and high utilization rate of catalysts. Besides the merits of nanotube arrays, the improved electrocatalytic activity and durability are especially attributed to the special Pd/PANI/Pd sandwich-like nanostructures, which results in electron delocalization between Pd d orbitals and PANI π-conjugated ligands and in electron transfer from Pd to PANI.
研究领域:
材料科学
·
电化学
·
纳米技术
·
能量转换
·
催化
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JOURNAL OF NANOBIOTECHNOLOGY
·
2023
·Vol. 21
·期 1
·1-22
·
IF 10.2
Zhang Shushan,Huang Yongquan,Pi Songying,Chen Hui,Ye Feile,Wu Chaoqun,Li Liujun,Ye Qing,Lin Yuhong,Su Zhongzhen
Incomplete radiofrequency ablation (IRFA) triggers mild protective autophagy in residual tumor cells and results in an immunosuppressive microenvironment. This accelerates the recurrence of residual tumors and causes resistance to anti-PD-1/PDL1 therapy, which bringing a great clinical challenge in residual tumors immunotherapy. Mild autophagy activation can promote cancer cell survival while further amplification of autophagy contributes to immunogenic cell death (ICD). To this regard, we constructed active targeting zeolitic imidazolate framework-8 (ZIF-8) nanoparticles (NPs) loaded with STF62247 or both STF62247 and BMS202, namely STF62247@ZIF-8/PEG-FA (SZP) or STF62247-BMS202@ZIF-8/PEG-FA (SBZP) NPs. We found that SZP NPs inhibited proliferation and stimulated apoptosis of residual tumor cells exposed to sublethal heat stress in an autophagy-dependent manner. Further results discovered that SZP NPs could amplify autophagy in residual tumor cells and evoke their ICD, which dramatically boosted the maturation of dendritic cells (DCs). Through vaccination experiments, we found for the first time that vaccination with heat + SZP treatment could efficiently suppress the growth of new tumors and establish long-term immunological memory. Furthermore, SBZP NPs could remarkably promote the ICD of residual tumor cells, obviously activate the anti-tumor immune microenvironment, and significantly inhibit the growth of residual tumors. Thus, amplified autophagy coupled with anti-PD-1/PDL1 therapy is potentially a novel strategy for treating residual tumors after IRFA.Graphical Abstract
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Environmental Science-Nano
·
2020
·Vol. 7
·期 7
·2117-2129
·
IF 7.683
Zhiqiang Zhang,Jinsuo Lu,Bing Zhang,Wenxin Shi,Yuan Guo,Fuyi Cui
Catalytic denitrification over Pd-based catalysts under mild conditions has received significant attention as an emerging technology. However, the Pd particle size effect has been much less systematically investigated. Herein, carbon-supported Pd nanoparticles (NPs) with particle sizes ranging from 2.1 to 22.1 nm were synthesized and characterized using high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), CO-chemisorption, and X-ray photoelectron spectroscopy (XPS). Catalytic nitrite reduction experiments were conducted in a semi-batch reactor at room temperature. The results showed that the highest mass catalytic activity of 603.6 mg gPd−1 min−1 was obtained at the Pd size of 2.7 nm. The turnover frequency (TOF) and the N2 selectivity increased gradually with the increasing Pd NP size. Considering both the mass catalytic activity and N2 selectivity, the Pd catalyst with a size of approximately 5 nm had a better comprehensive performance. Mechanism studies showed that the enhanced TOF of larger Pd NPs could be ascribed to the formation of more β-hydride, which has a higher reducing activity than α-hydride. Compared with the terraces, the edges and corners of Pd NPs are the major active sites where ammonia is generated, most likely because of their low-coordination and electron-deficient properties. This indicated that the NO2− catalytic reduction is a size sensitive reaction in terms of both activity and selectivity, and may provide new insight into tailoring Pd NP size of Pd-based catalysts to improve catalytic activity and selectivity for nitrate and nitrite reduction in water.
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