ACS Nano
·
2024
·
IF 15.8
Shizhen Geng,Pengke Guo,Xinling Li,Yaru Shi,Jing Wang,Mengnian Cao,Yunya Zhang,Kaixiang Zhang,Airong Li,Haiwei Song,Zhenzhong Zhang,Jinjin Shi,Junjie Liu,Yiling Yang
Immune checkpoint blockade (ICB) therapy has been approved for breast cancer (BC), but clinical response rates are limited. Recent studies have shown that commensal microbes colonize a variety of tumors and are closely related to the host immune system response. Here, we demonstrated that Fusobacterium nucleatum (F.n), which is prevalent in BC, creates an immunosuppressive tumor microenvironment (ITME) characterized by a high-influx of myeloid cells that hinders ICB therapy. Administering the antibiotic metronidazole in BC can deplete F.n and remodel the ITME. To prevent an imbalance in the systemic microbiota caused by antibiotic administration, we designed a biomimetic nanovehicle for on-site antibiotic delivery inspired by F.n homing to BC. Additionally, ferritin-nanocaged doxorubicin was coloaded into this nanovehicle, as immunogenic chemotherapy has shown potential for synergy with ICB. It has been demonstrated that this biomimetic nanovehicle can be precisely homed to BC and efficiently eliminate intratumoral F.n without disrupting the diversity and abundance of systemic microbiota. This ultimately remodels the ITME, improving the therapeutic efficacy of the PD-L1 blocker with a tumor inhibition rate of over 90% and significantly extending the median survival of 4T1 tumor-bearing mice.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Zhiang Hou,Hao Chen,Jiangfeng Chu,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Herein, the bimetallic Pd 3 In 1 alloy were deposited onto the crystal facet engineered TiO 2 nanosheet (NS) via one-step photoreduction (Pd 3 In 1 /TiO 2 -NS) for selective conversion of nitrate (NO 3 − ) to N 2 . Bimetallic Pd 3 In 1 provides higher affinity sites to bind NO 3 − and significantly reduces the energy barrier of the rate-limiting step (NO 3 * + e − → NO 2 *), which is the key for the ultra-fast NO 3 − reduction kinetics. More importantly, the synergistic effect of Pd and In not only suppresses the hydrogen evolution reaction resulting in high efficiency utilization of photogenerated electrons, but also promotes the selective conversion of nitrite (NO 2 − ) to N 2 . Consequently, Pd 3 In 1 /TiO 2 -NS exhibits 100 % NO 3 − conversion and 90 % N 2 selectivity within 20 min in six cycles. One order of magnitude improvement on the NO 3 − reduction kinetic constants of Pd 3 In 1 /TiO 2 -NS (0.254 min −1 ) is achieved compared with pristine TiO 2 -NS and monometallic loaded ones. This work provides new insights into the rational construction of bimetallic alloy cocatalysts for high-efficiency photocatalytic denitrification.
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JOURNAL OF MATERIALS CHEMISTRY
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2012
·Vol. 22
·期 18
·9117-9122
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IF 5.968
Sha Chen,Hongye Zhang,Lingyan Wu,Yanfei Zhao,Changliang Huang,Maofa Ge,Zhimin Liu
Based on the galvanic replacement reaction between Cu nanoparticles and noble metal ions, a simple and efficient strategy was developed for the preparation of supported Cu–M (M = Pt, Pd, Ru, Rh) bimetallic nanoparticles under intense ultrasonication irradiation at ambient environment. A series of Cu–M/TiO2 bimetal catalysts with controllable composition, metal particle size less than 2 nm and narrow size distribution were obtained, and characterized by transmission electron microscopy (TEM), high resolution transmission electron microscope (HRTEM) with scanning TEM (STEM) mode, energy-dispersive X-ray spectrometers (EDS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and ICP-AES analysis. It was demonstrated that most of the metal particles were present in the form of bimetallic state. The mechanism of this strategy was discussed. The resultant Cu–Pd/TiO2 was used to reduce nitrate at room temperature, and it exhibited extremely high activity.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2017
·Vol. 22
·期 3
·817-824
·
IF 2.316
Liu Yong,Li Shenshen,Zhang Yunmao,Liu Weihua,Wang Jianhong,Zhai Cuiping
Honeycomb-like porous carbons (PCs) were synthesized using a facile self-assembly method with phenolic resin as the carbon source and tetraethyl orthosilicate (TEOS) as the silica source. The PCs were found to have a large BET surface area of 458 m 2 g −1 and a partially graphitized structure. The obtained PCs were used as a support for various Pt-Pd bimetallic alloy catalysts employed for methanol oxidation in alkaline media. Compared with Pt supported on commercial Vulcan XC-72R carbon (Pt/C) and with the other Pt-Pd bimetallic alloy catalysts on PCs, Pt 3 Pd 1 on PCs displayed the most negative onset potential for methanol oxidation and the highest steady-state current (2.04 mA cm −2 ). This may be because the Pt 3 Pd 1 /PCs catalyst has the largest electrochemical active surface area (ESA), and because adding Pd to the catalyst improves the ability of the intermediate species to tolerate oxidation. The results show that the prepared Pt-Pd/PCs is a potential candidate for application as a catalyst in alkaline direct methanol fuel cells.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Hu Li,Wenfeng Zhao,Zhen Fang
Liquid furanic hydrocarbons, a class of biomass-based fuels and chemicals, are typically required to achieve moderate product selectivity and yield under harsh conditions (e.g., high temperature and H 2 pressure) involving multi-step processes over different catalysts. In this study, a single-step catalytic process was developed for direct conversion of various saccharides to furanic biofuels such as 2,5-dimethylfuran and 2-methylfuran with high yields (>95%) at 110–130 °C. The negatively charged hydride (H − ) of readily available polymethylhydrosiloxane (PMHS) acting as green H-donor over hydrophobic Pd nanoparticles did not obstruct upstream reactions (e.g., hydrolysis, isomerization and dehydration) for the in situ formation of furanic aldehydes/alcohols from sugars, and could selectively facilitate the subsequent hydrodeoxygenation of carbonyl and hydroxyl groups other than the furanic ring in one pot, as clarified by deuterium-labeling study. Importantly, the unreduced Pd(II) nanocatalysts also exhibited comparable performance in the selective hydrodeoxygenation reaction. Moreover, the catalytic strategy was extended to various carboxides for quantitative production of corresponding furanic/aromatic hydrocarbons at room temperature that were more pronounced than previously reported results, and the optimal Pd/MIL-53(Al) coated with polydimethylsiloxane (Pd/MIL-53(Al)-P) was highly stable with little deactivation and Pd leaching for at least five consecutive cycles.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2024
·Vol. 25
·期 7
·3735
·
IF 4.9
Jing Sun,Zhengtian Zhao,Jiaqi Lu,Wen An,Yiming Zhang,Wei Li,Li Yang
The unsatisfactory efficacy of immunotherapy for colorectal cancer (CRC) remains a major challenge for clinicians and patients. The tumor microenvironment may promote CRC progression by upregulating the expression of hypoxia-inducing factor (HIF) and PD-L1. Therefore, this study explored the expression and correlation of HIF-1α and PD-L1 in the CRC microenvironment. The expression and correlation of HIF-1α and PD-L1 in CRC were analyzed using bioinformatics and Western blotting (WB). The hypoxia and inflammation of the CRC microenvironment were established in the CT26 cell line. CT26 cells were stimulated with two hypoxia mimics, CoCl2and DFO, which were used to induce the hypoxic environment. Western blotting was used to assess the expression and correlation of HIF-1α and PD-L1 in the hypoxic environment.LPS stimulated CT26 cells to induce the inflammatory environment. WB and bioinformatics were used to assess the expression and correlation of TLR4, HIF-1α, and PD-L1 in the inflammatory environment. Furthermore, the impact of curcumin on the inflammatory environment established by LPS-stimulated CT26 cells was demonstrated through MTT, Transwell, molecular docking, network pharmacology and Western blotting assays. In this study, we found that the HIF-1α/PD-L1 pathway was activated in the hypoxic and inflammatory environment and promoted immune escape in CRC. Meanwhile, curcumin suppressed tumor immune escape by inhibiting the TLR4/HIF-1α/PD-L1 pathway in the inflammatory environment of CRC. These results suggest that combination therapy based on the HIF-1α/PD-L1 pathway can be a promising therapeutic option and that curcumin can be used as a potent immunomodulatory agent in clinical practice.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Fei Dou,Fengchen Guo,Bo Li,Kai Zhang,Nigel Graham,Wenzheng Yu
Electro-catalytic conversion of nitrate (NO 3 - ) to ammonia (NH 3 ) via the Nitrate Reduction to Ammonia (NORA) process represents a promising strategy for both ammonia synthesis and environmental remediation. Despite its potential, the efficiency of low-concentration NORA is often hindered by mass transfer limitations, competing byproducts (N 2 and NO 2 - ), and side reactions such as hydrogen evolution . This study introduces a novel pulsed electro-synthesis technique that alternates the potential to periodically accumulate and transform NO 2 - intermediates near a Cu2O@Pd electrode, enhancing the NORA process. Compared with that under potentiostatic conditions, the Cu 2 O@Pd electrodes exhibited a higher NORA activity under the optimized pulsed condition, where a NH 3 -N Faradaic efficiency (FE) of 81.2%, a yield rate of 1.08 mg h -1 cm -2 and a selectivity efficiency (SE) of 81.5%, were achieved. In-situ characterization revealed an enhancement mechanism characterized by optimized adsorption of the key *NO intermediate, followed by the hydrogenation path “*N → *NH → *NH 2 → *NH 3 ”. Further investigations indicated the electro-catalytic synergies between Pd sites and Cu species, where the Pd atoms were the reaction sites for the H adsorption while the Cu species were responsible for the NO 3 - activation. This research offers a novel insight into a method of enhancing low-concentration NORA.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yacong Yang,Zhihao Cao,Tianhan Shen,Junyang Zhang,Zuofei Gu,Mingwan Zhao,Zongli Xie,Yingchun Miao,Yuning Huo,Hexing Li
The photocatalytic membrane systems show great potential for water purification and wastewater treatment with efficient energy utilization. Herein, we develop a synergistic photocatalytic-photothermal route, based on Pd-TiO 2 /PEDOT composite immobilized in PVDF membrane, for effective water permeability and reutilization property. Novel Pd-TiO 2 /PEDOT/PVDF ultrafiltration membrane is prepared by the phase inversion method with immobilizing Pd-TiO 2 /PEDOT obtained by ultrasonic irradiation. During the removal of HA under light irradiation, Pd-TiO 2 /PEDOT/PVDF membrane presents an unexpected increasing in water flux, when compared to pristine PVDF, Pd-TiO 2 /PVDF and PEDOT/PVDF membranes, with the highest normalized flux reaches up to 2.1 and remains as 1.3 even after 300 min of irradiation. This significantly enhances the water transport, along with the achieved high rejection and anti-fouling performance. It can be attributed to synergistic photocatalytic-photothermal effect of Pd-TiO 2 /PEDOT, which is realized by their strong interaction and uniform distribution. The addition of PEDOT promotes photocatalytic effect of Pd-TiO 2 by enhancing separation of photo-induced charges. High photothermal conversion efficiency of Pd-TiO 2 /PEDOT and low temperature difference in Pd-TiO 2 /PEDOT/PVDF membrane facilitate effective thermal storage, beneficial for water transport. Meanwhile, thermal energy promotes generation of more ∙OH and ∙O 2 – radicals to remove pollutants. Synergistic photocatalytic-photothermal contribution in Pd-TiO 2 /PEDOT/PVDF membrane shows significant potential for practical application.
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LANGMUIR
·
2025
·
IF 3.9
Peng Guo,HongWei Li,BoYu Huang,Dong Ji,GuiXian Li,XinHong Zhao
Despite nitrogen-doped carbons (NC) enhancing metal–support interactions (MSI) in electrocatalysts, how specific N-configurations (pyridinic, pyrrolic, and graphitic) synergistically govern methanol oxidation reaction (MOR) pathways over Pd surfaces remains unknown. Herein, we hypothesize that precise thermal programming of ZIF-8 pyrolysis can tailor synergistic pyridinic-pyrrolic-graphitic N-triads to simultaneously enhance activity, CO tolerance, and stability. Guided by DFT predictions, Pd/NC-T catalysts (T = 700–1100) were synthesized, where in situ pyrolysis controls N-configurations (validated by XPS) and wet impregnation immobilizes ultrafine Pd nanoparticles (3.6 ± 0.8 nm). Furthermore, experimental and theoretical analyses reveal that pyrrolic-N facilitates the adsorption of methanol on Pd, while pyridinic-N suppresses the CHO* → CO* reaction pathway, thus enhancing the catalyst’s tolerance to poisoning, and graphitic-N prevents support dissolution and collapse during the electrocatalytic reaction, thus mitigating active site loss. Notably, Pd/NC-900 achieves 4195.0 mA·mg–1Pd in the alkaline electrolyte, maintaining 80.5% of its initial current density after 500 cycles at 200 mV/s, highlighting its exceptional catalytic activity and long-term stability. This work offers profound insights into the intricate MSI, serving as a crucial framework for guiding the future design and advancement of MOR electrocatalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Ertai Na,Binrong Chen,Xudong Liang,Jiayu Li,Ruiqin Gao,Xu Zou,Guo-Dong Li
n -Butanol, as a typical volatile organic compound, is widely used in the chemical, coating, and daily chemical industries. However, its volatility can lead to deteriorating air quality and health risks, necessitating the development of highly sensing and selective real-time detection sensors. This investigation proposes a synergistic sensitization strategy by modifying ZnO nanosheets with Pd nanoparticles to address the low response and poor selectivity of traditional ZnO semiconductor gas-sensing materials. Experimental results indicate that the 0.25 wt% Pd-ZnO exhibits a response value of 400 for 50 ppm of n -butanol, which is seven times that of pure ZnO, and the detection limit is as low as 0.1 ppm. Combined with density functional theory calculations, we reveal for the first time the synergistic sensing-enhancement mechanism at the Pd-ZnO interface: the Zn sites adsorb the oxygen atoms in n -butanol through bonding interactions, while the Pd nanoparticles can synergistically adsorb the hydrogen atoms in n -butanol, thereby enhancing the specific recognition capability towards n -butanol. This research provides new insights into the sensing enhancement mechanisms of noble metal-modified semiconductors, these insights may be widely applied in the design and synthesis of specific sensing materials, catalytic materials, and adsorption materials.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Jinqiang Fu,Fenglan Liang,Wenjing Zhong,Tao Kuang,Ziyuan Yin,Yongshi Li,Zhenggui Huang,Hongli Liu,Deyun Ma
Establishing a simple and consistent strategy to adjust the photocatalyst surface to improve the photocatalytic performance is crucial but remains challenging. Herein, a photocatalyst of TiO 2 -Q-Pd is obtained through one-step quenching of TiO 2 (derived from NH 2 -MIL-125(Ti)) into an aqueous solution of sodium tetrachloropalladium, which displayed a significant improvement in photocatalytic activity, achieving 97 % tetracycline degradation within 60 min and 95 % mineralization at 5 h. The mineralization reaction rate (0.6321 h −1 ) was 2.75 times that of the commercial TiO 2 . Our findings show that quenching leads to the creation of numerous zigzag surfaces and the near-surface palladium atom doping, therefore adjusting the chemical environment of Ti, which accelerates electron-hole pair separation and transfer, and thereby improves the photocatalytic performance. This finding introduces a novel approach to activating metal oxide catalysts derived from MOFs and expands the role of quenching chemistry in catalytic processes.
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Molecular Catalysis
·
2025
·
IF 4.9
Long-Gen Hu,Guo-Sheng Zhang,Guang-Hui Shi,Jian-Guo Qian,Hai-Jing Wang,Ye Liu
The Pd-catalyzed aminocarbonylation as well as hydroxycarbonylation of terminal alkynes was achieved with aid of a sulfonate-built-in zwitterionic phosphine ( L2 ), under acid-additive free condition. With L2 -Pd(OAc) 2 catalytic system, the terminal alkynes smoothly converted to the corresponding α,β -unsaturated carbonyl compounds (amides or carboxylic acids) in moderate to excellent isolated yields, with 100 % branched regio-selectivity. It was believed that L2 with the matched steric-demand and the bulit-in-SO 3 - -unit not only tuned the catalytic performance of Pd(OAc) 2 to activate CO and alkyne but also exhibited the synergetic activating ability towards the nucleophiles of (primary/secondary) amines or H 2 O via developing hydrogen-bond interaction, which facilitated the observed successful carbonylation. It means the developed L2 -Pd(OAc) 2 system could serve as a bifunctional catalyst.
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