Electrocatalysis
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2025
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IF 2.8
Gao Hongmin,Deng Jiahe,Zhang Hehua,Chen Hua,Zhou Yang,Qu Pu,Zhu Huan,Chang Dong,Pan Hongzhi
Developing portable, accurate, cost-effective hydrogen peroxide (H 2 O 2 ) detection platforms is essential for industrial applications and early disease diagnosis. Metal–organic frameworks (MOFs) based composites integrated with metal nanoparticles have been intensively investigated in electrochemical sensing, attributable to their unique architecture and performance characteristics. Herein, PdNPs@NH 2 -MIL-101(Fe) nanocomposites were synthesized via a green reduction process using tannic acid and applied in the development of an enzyme-free electrochemical sensor for H 2 O 2 detection. The synergistic effect of the Pd nanoparticles and the MOFs matrix provided abundant active sites and enhanced electron transfer capability, enabling the sensor to exhibit excellent electrocatalytic performance. Under optimal conditions, the sensing platform exhibited a wide linear response from 10 μM to 15 mM, with a detection threshold of 3.6 μM (S/N = 3). Furthermore, the sensor achieved reliable detection of exogenous H 2 O 2 in commercial mouthwash samples and intracellularly generated H 2 O 2 by cancer cells (HepG2), underscoring its effectiveness in practical scenarios. This work presents a novel strategy for synthesizing high-performance composite nanomaterials and offers valuable insights into the large-scale application of electrochemical sensors for H 2 O 2 detection. Graphical
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yingying Zhao,Beibei Zhang,Shaobo Duan,Yaqiong Li,Yuzhou Wang,Yongchao Wang,Juan Zhang,Rong Huang,Ru Jiang,Rui Zhang,Qi Zhou,Linlin Zhang,Xiaoxia Xu,Zesheng Li,Si Chen,Lianfeng Mo,Xu Zhang,Siyi Yang,Xiguo Cai,Lianzhong Zhang
Metabolic competition and accumulation of metabolic byproducts in the tumor microenvironment (TME) severely impair the antitumor functions of T cells, leading to suboptimal outcomes in cancer immunotherapy. To address these challenges, we developed an ultrasound-visualized methionine partitioning nano-modulator utilizing erythrocyte membrane-hybridized liposomes loaded with the glycolysis inhibitor lonidamine (LND) and small interfering RNA (siRNA) against methionine transporter solute carrier family 43, member 2 (SLC43A2). By downregulating SLC43A2 expression to reduce methionine uptake by tumor cells and suppressing tumor glycolysis to alleviate the acidic TME, the nano-modulator enhances methionine availability for T cells and improves T cell activity. Moreover, the oxygen-enriched perfluorohexane (PFH-O 2 ) loaded in the core of the nano-modulator alleviates tumor hypoxic, further reducing the glycolysis rate of tumor cells. Furthermore, ultrasound-triggered liquid-gas phase transitions enable real-time ultrasound contrast imaging for precise tumor visualization, while leveraging the ultrasonic cavitation effect to enhance drug penetration and release at the tumor site. In summary, this ultrasound-visualized methionine partitioning nano-modulator effectively reshapes tumor metabolism and immunosuppressive TME under ultrasound guidance, thereby significantly improving the efficacy of tumor immunotherapy. These findings demonstrate a promising strategy for enhancing immunotherapy outcomes through metabolic modulation and microenvironment regulation.
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Nature Communications
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2025
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IF 15.7
Su Keying,Yang Shan,Liang Yujia,Sun Dongmei,Gong Mingxing,Tang Yawen,Qiu Xiaoyu
Single-atom catalysts are highly active for specific reactions; however, their sinter-resistance and clean surfaces make it difficult to impart them with a “smart” property. Herein we design a thermosensitive single-atom Rh 1 -Pd nanosheets (NSs) by employing amino functionalized poly( N -isopropylacrylamide) as thermal responsive gate for the “open”/“closed” control of electro-catalytic activity. Using formic acid electro-oxidation as model reaction, the thermosensitive Rh 1 -Pd NSs exhibit high mass activity (2.29 A mg PGM -1 ), strong poisoning resistance, and reversible thermo-responsibility at a lower critical solution temperature (LCST) of 35 o C. In-situ spectroscopy and theoretical investigations reveal that the d-electron deficient Rh 1 -Pd NSs favor the direct formate pathway and weaken the binding of self-poisonous species, contributing to the high activity and anti-self-poisoning talent. Most importantly, for the direct formic acid fuel cells (DFAFCs), the thermosensitive Rh 1 -Pd NSs exhibit a high power density operated below the LCST, while the power drops sharply once above the LCST, realizing the intelligent battery thermal protection for DFAFCs.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Yakai Chen,Xinya Feng,Xiaohan Yu,Xingliang Xu,Jing Xu
Catalytic transfer hydrogenation of nitro compounds to amines under mild conditions offers an alternative strategy to traditional hydrogenation processes involving pressurized molecular hydrogen, which necessitate the rational design and integration of multifunctional catalyst. Herein, a ternary composite catalyst (Pd/CeO 2 -C 3 N 4 ) was designed and synthesized for the transfer hydrogenation of nitro compounds to corresponding amines compounds using formic acid as hydrogen donor. The Pd/CeO 2 -C 3 N 4 catalyst shows remarkably high performance for the catalytic transfer hydrogenation of nitrobenzene (NB) to aniline (BA), achieving > 98 % conversion and exceedingly high selectivity (>99 %). The catalyst exhibits a high turnover frequency (TOF) of up to 2868 h - , significantly surpassing both the reference catalyst (Pd/C 3 N 4 and Pd/CeO 2 ) and the conventional Pd/C catalyst. The multi-functional Pd/CeO 2 -C 3 N 4 catalyst features enhanced electron transfer properties,well-exposed Pd active sites, and abundant acid-base sites, enabling effective enhancement of formic acid dehydrogenation and nitro group activation. Moreover, Pd/CeO 2 -C 3 N 4 demonstrates excellent recyclability and a broad substrate scope for the catalytic transfer hydrogenation of various nitro compounds. The rational design of Pd/CeO 2 -C 3 N 4 will broaden the application range of Pd-based catalysts and provide a sustainable and effective approach for the catalytic transfer hydrogenation of other industrially relevant organic compounds.
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Translational Cancer Research
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2025
·Vol. 14
·期 10
·6454
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IF 1.7
Jiaxuan Zhao,Han Wu,Zhe Sun,Yeting Cui,Nan Liu,Yixuan Wang,Youyong Wang,Jiangzhou Shi,Tongcun Zhang
Background Chimeric antigen receptor T cell (CAR-T) therapy targeting cluster of differentiation 19 (CD19) has shown promise in treating B-cell acute lymphoblastic leukemia (B-ALL), but the long-term efficacy of CD19-targeted CAR-T therapy remains limited. Programmed cell death protein 1 (PD-1), an inhibitory receptor on activated T cells, engages programmed death ligand 1 (PD-L1) in the tumor microenvironment, suppressing CAR-T cell function by impairing key signaling pathways. To address this limitation, we investigated the effect of short hairpin RNA (shRNA)-mediated PD-1 knockdown on alleviating CAR-T cell exhaustion, preserving memory phenotype, and enhancing the long-term efficacy of CD19-targeted CAR-T cells. Methods To overcome this limitation, we employed shRNA to achieve PD-1 knockdown in CD19-targeting CAR-T cells. Following screening multiple shRNA candidates, we assessed the cytotoxicity, cytokine secretion, and proliferation of PD-1 knockdown CAR-T cells. Their memory phenotype, exhaustion marker, and cytolytic function were further evaluated after repeated antigen stimulation. Therapeutic efficacy and safety were validated in NOD.Cg-PrkdC scid Il2rg tm1 /Vst (NPG) mice. Results PD-1 knockdown significantly enhanced CAR-T cell cytotoxicity and persistence against PD-L1+ RAJI (human Burkitt’s lymphoma cell line) cells. After three rounds of antigen stimulation, PD-1 knockdown CAR-T cells sustained cytotoxic activity, retained a memory-like phenotype, and displayed attenuated exhaustion markers. In vivo , they prolonged survival without inducing cytokine release syndrome (CRS), indicating improved efficacy and safety. Conclusions PD-1 knockdown mitigates tumor-induced T-cell exhaustion and represents a promising strategy to enhance the durability and potency of CAR-T cell therapy in cancer treatment.
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Ecological Frontiers
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2025
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IF 0
Xinyi Wu,Yan Li,Linghan Li,Hongwei Liu,Yongguang Yin,Shixiang Gao,Maoyong Song,Zhiqiang Tan,Yan Ma
Monitoring nanoplastic (NP) aggregation in bidisperse systems under environmentally relevant ionic conditions remains a significant challenge. Conventional techniques such as dynamic light scattering and transmission electron microscopy are hindered by matrix interference, low sensitivity, and difficulties in resolving polydispersity. Here, we addressed this gap by using a coupled system including hollow fiber flow field-flow fractionation (HF5), ultraviolet-visible detector (UV), and point-discharge optical emission spectroscopy (PD-OES) to investigate aggregation behavior of bidisperse polystyrene NPs (PSNPs, 50 nm and 100 nm) at ionic conditions below 1 mM, representative of freshwater ecosystems. We demonstrated that bidisperse PSNPs exhibit enhanced aggregation compared to monodisperse counterparts by using the HF5-UV/PD-OES platform for purification, separation, and carbon-specific quantification. This platform elucidated the critical roles of cation valence (Na + vs. Ca 2+ ) and low concentration ion gradients (0.01–1 mM) in modulating aggregation over extended scales (i.e., 24 h). Finally, toxicity assessments on Microcystis aeruginosa revealed that aggregation reduces PSNP ecotoxicity depending on cation valence, thereby alleviating growth inhibition, oxidative stress, and impairment of chlorophyll biosynthesis. These findings elucidate how environmentally relevant ionic conditions govern NP fate and effects in freshwater ecosystems, providing a critical link between physicochemical transformations and biological responses for ecological risk evaluation.
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Green Energy & Environment
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2025
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IF 14.6
Wen Zhao,Qun Yu,Bingqing Wei,Lei Nie,Fabio Souza Toniolo,Zhenglong Li
Although current methods enable lignin extraction and depolymerization, the selective hydrogenolysis of lignin into alkene-functionalized monomers remains a significant scientific challenge. These monomers can be further functionalized into diverse natural products or pharmaceutical intermediates, thereby enabling higher-value utilization of biomass resources. Here, we report a catalyst with low Pd loading (0.4 wt%) supported on ZnO-modified carbon nanotubes (Pd/ZnNC) for the selective catalytic hydrogenolysis of the dimer β-O-4 lignin model compound (veratrylglycerol-β-guaiacyl ether, VG) via distinct reaction pathways. The Pd/ZnNC catalyst achieves a selectivity of 37.5% toward alkene-functionalized monomers (1,2-dimethoxy-4-allylbenzene and 1,2-dimethoxy-4-propenylbenzene), approaching 75% of the theoretical maximum selectivity (50%). In contrast, the Pd/CNT catalyst predominantly produces 3-(3,4-dimethoxyphenyl)-1-propanol, and excessive side-chain saturation of monomers are not conducive to subsequent utilization processes. Moreover, the Pd/ZnNC catalyst achieves a conversion rate seven-fold higher than that of commercial catalysts Pd/C (5 wt%). Experimental characterization results demonstrate that the ZnO sites on carbon nanotubes facilitate the dispersion of Pd nanoparticles, resulting in a reduction in particle size. Furthermore, the synergistic effect between ZnO and Pd active sites promotes the selective catalytic formation of monomers containing unsaturated C=C bonds. The DFT calculations reveal that the Cγ-OH elimination is facilitated by Pd nanoparticles supported on ZnO, which reduces the reaction energy barrier and promotes the generation of propenyl-substituted monomers. The pathway enabled by Pd/ZnNC catalyst offers a great potential for lignin depolymerization into high-value products.
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Frontiers in Bioengineering and Biotechnology
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2023
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IF 5.7
Wei Min,Shen Xiao,Fan Xueqi,Li Jiwei,Bai Jingwen
Immune checkpoint blockade is now recognized as a paradigm-shifting cancer therapeutic strategy, whereas there remains difficulty in accurately predicting immunotherapy efficacy by PD-L1 expression. In addition, radiotherapy for cancer patients faces the problem of insufficient dose of radiotherapy at the tumor site while which have been not tolerated by normal tissues. In this study, we created PD-L1 aptamer-anchored spherical nucleic acids (SNAs) with a shell made of PD-L1 aptamer and indocyanine green (ICG) embedded in a mesoporous hafnium oxide nanoparticle core (Hf@ICG-Apt). Upon low pH irradiation in the tumor sites, the nano-system enabled the release of ICG in the high PD-L1 expression tumor to develop a high tumor-to-background ratio of 7.97 ± 0.76 and enhanced the ICG tumor retention to more than 48 h. Moreover, Hf@ICG-Apt improved radiation therapy (RT) when combined with radiation. Notably, Hf@ICG-Apt showed scarcely any systemic toxicity in vivo. Overall, this research offered a novel approach for applying reliable monitoring of PD-L1 expression and localization and robust RT sensitization against cancer with good biosafety.
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ANALYTICAL CHEMISTRY
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2019
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IF 6.35
Shuzhen Lv,Kangyao Zhang,Ling Zhu,Dianping Tang,Reinhard Niessner,Dietmar Knopp
With the introduction of gas-based contactless electrochemical biosensors lies the prospects of separating the sensing interface from the bioassembly platform, enhancing stability, and exploring signal transduction mechanism, all intimately linking to development of immunoassay. Herein, we report on a H2-based electrochemical biosensor whose signals derived from the chemical signal transduction between a H2 and Pd nanowires@ZIF-67 (ZIF: Zeolitic Imidazolate Frameworks) bilayered sensing interface for immunoassay. Dendritic Pt nanoparticles (DPNs) conjugated on the detection antibody were introduced on the interface of a magnetic microsphere according to an immune sandwich assembly between the antigen and antibody. H2 as a bridge originates from DPNs catalyzing NH3BH3 and links biological signals to electrical signals by reacting with Pd nanowires. Nevertheless, the response of Pd nanowires being extremely effected by O2 in air due to the competitive adsorption on the surface of Pd nanostructures as well as the reaction between chemisorbed O (Pd–O) and adsorbed dihydrogen lead to a decrease in H absorption into PdHx and poor sensing responses under low target concentration. Porous ZIF-67 (window aperture 0.331 nm) as a molecular sieve self-assembling on the surface of the Pd nanowires film could easily permeate H2 (kinetic diameter of 0.289 nm), while interferential O2 (kinetic diameter of 0.346 nm) has difficultly passing through the ZIF-67 layer to contact Pd nanowires and achieves a response of a lower concentration target as well as faster response rate. Under optimal conditions, H2-based electrochemical biosensors exhibit great response toward target alpha-fetoprotein (AFP) within a dynamic working range of 0.1–50 ng mL–1 at a detection limit of 0.04 ng mL–1. Our strategy provides a reusable sensing interface, high specificity, and acceptable accuracy for the immunoassay. In addition, it also expands a promising platform for application as a molecular sieve in electrochemical biosensors.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
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2017
·Vol. 314
·期 1
·59-67
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IF 1.282
Liu Zhanxiang,Dong Yang,Liao Jiali,Li Xingliang,Yang Jijun,Yang Yuanyou,Luo Shunzhong,Liu Ning
A novel extractant, 5-octyloxymethyl-7-bromo-8-quinolinol (HBrO 8 Q), was employed to extract Pd(II) from low-acidity aqueous solution. The extraction behaviors indicated that HBrO 8 Q had high extraction efficiency and selectivity for Pd(II) under the experimental conditions, and the stoichiometry of Pd(II) with HBrO 8 Q was found to be 1:1 by means of mole ratio method and Job’s method. The thermodynamic study indicated that the extraction process was endothermic and spontaneous. Additionally, complete back extraction of palladium could be achieved by using acidic thiourea solution.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2026
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IF 9.2
Yifan Yang,Lu Jin,Guoxiang Chen,Jiabao Ye,Yongfeng Mei
A transparent nanoporous Pd-WO 3 -Nafion film is developed for gasochromic H 2 leak detection. • The Nafion overlayer significantly boosts the transmittance variation and response kinetics. • A semi-enclosed attachable H 2 leak detector with a top vent ensures the safe upward release of H 2 . • The reusable and detachable detector allows precise visual localization of leaks in H 2 systems. Hydrogen (H 2 ) is a promising clean energy carrier, but its high leakage risk and explosive nature demand safe and reliable detection technology. Here, we present a reusable and attachable H 2 leak detector based on a transparent gasochromic Pd-WO 3 -Nafion film. The film consists of a nanoporous WO 3 layer decorated with an ultrathin Pd (2 nm) catalyst and a Nafion overlayer. It exhibits a transmittance variation of approximately 59% (from 75% to 16%) upon exposure to 4% H 2 , with a coloring time of 69 s and a bleaching time of 117 s. Notably, the Nafion coating significantly enhances the transmittance variation and response kinetics compared to Nafion-free films. Building on this material, we design a semi-enclosed detector with a top vent for safe upward H 2 release and clear visual detection. Its detachable configuration enables repeated use and precise leak localization across complex systems, providing a cost-effective, visually intuitive solution for H 2 infrastructure. Download: Download high-res image (214KB) Download: Download full-size image
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ACS Omega
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2021
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IF 3.512
Lin-Xi Wan,Yong-Qi Zhen,Zhen-Xiang He,Yang Zhang,Lan Zhang,Xiaohuan Li,Feng Gao,Xian-Li Zhou
A new series of N-aryltacrine derivatives were designed and synthesized as cholinesterase inhibitors by the late-stage modification of tacrine, using the palladium-catalyzed Buchwald–Hartwig cross-coupling reaction. In vitro inhibition assay against acetylcholinesterase (AChE) and butyrylcholinesterase (BuChE) demonstrated that most of the synthesized compounds had potent AChE inhibitory activity with negative inhibition of BuChE. Among them, N-(4-(trifluoromethyl)phenyl)-tacrine (3g) and N-(4-methoxypyridin-2-yl)-tacrine (3o) showed the most potent activity against AChE (IC50 values of 1.77 and 1.48 μM, respectively). The anti-AChE activity of 3g and 3o was 3.5 times more than that of tacrine (IC50 value of 5.16 μM). Compound 3o also displayed anti-BuChE activity with an IC50 value of 19.00 μM. Cell-based assays against HepG2 and SH-SY5Y cell lines revealed that 3o had significantly lower hepatotoxicity compared to tacrine, with additional neuroprotective activity against H2O2-induced damage in SH-SY5Y cells. The advantages including synthetic accessibility, high potency, low toxicity, and adjunctive neuroprotective activity make compound 3o a new promising multifunctional candidate for the treatment of Alzheimer’s disease.
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