CHEMICAL ENGINEERING JOURNAL
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2024
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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
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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
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2025
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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
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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
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2025
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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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ADVANCED MATERIALS
·
2025
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IF 26.8
Xiejun Zhao,Xiangchuan Qin,Ruizhe Wang,Yawen Wang,Yinli He,Yuchen Wang,Kefeng Li,Peipei Zhang,Chen Yang,Menghan Wang,Yingtong Dong,Xue Shi,Jia Ma,Jiye Zhang,Xiaojiao Li
Inefficient priming, poor recruitment, and inadequate reinvigoration of T cells challenges the therapy of PD-L1-resistant tumors. Herein, a pH-responsive charge-reversal nanoplatform integrating coactivator-associated arginine methyltransferase 1 (CARM1) inhibitor (iCARM1) and poliovirus receptor siRNA (siPVR) is developed. Upon tumor penetration, iCARM1 released in tumor cells facilitates T cell priming by epigenetically activating cyclic GMP-AMP synthase (cGAS)-stimulator of interferon genes (STING) signaling-mediated dendritic cell maturation. Meanwhile, in T cells, iCARM1 facilitates their recruitment by upregulating CXC-chemokine receptor 3 (CXCR3) expression. The released siPVR silences pvr to reinvigorate T cells. This epigenetic nanoagonist induces a robust immune response, dramatically suppresses tumor growth, metastasis, and relapse, and confers durable protection against secondary tumor challenge. Multiple PD-L1-resistant models demonstrate the broad applicability of this strategy. This study thus represents an innovative approach for facilitating multilevel T cell responses to combat PD-L1-resistant tumors.
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BIOMATERIALS
·
2025
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IF 12.9
Zhanxue Xu,Xinrui Yang,Xingyu Lu,Dandan Su,Yidan Wang,Huixing Wu,Zhenhua Zhang,Changrui Long,Liqian Su,Yanyu Wang,Hongbo Chen,Shijian Xiang,Benjie Zhou
Combination therapies for melanoma face challenges due to asynchronous drug delivery and associated toxicity, underscoring the need for advanced delivery systems. While immune checkpoint inhibitors (ICIs) enhance T cell activity, optimal cytotoxic responses require efficient antigen presentation by mature dendritic cells (DCs), which are often functionally impaired in the tumor microenvironment. Thus, effective treatment requires coordinated T cell activation, DC-mediated priming, and direct tumor suppression. Herein, wild Glycyrrhiza uralensis Fisch roots-derived nanovesicles (GC NV) are demonstrated to be effective inhibitors of melanoma proliferation. The vesicles exert this activity through the intracellular delivery of encapsulated miRNA (miR2916) and bioactive molecules (isoliquiritigenin), with this capacity for intracellular delivery extending to the STING agonist DMXAA. We also demonstrate how chemical modification can be used to install PD-L1 antibodies on the membrane surface of these GC NV, imbuing these vesicles with selectivity for tumor cells. Combining DMXAA encapsulation with surface-displayed PD-L1 antibodies creates vesicles (GP@DMX NV) that both promote DCs maturation and elicit CD8 + T cell response. Our multifunctional GP@DMX NV reverse the immunosuppressive microenvironment of melanoma and significantly enhance the immunotherapeutic potential of immune checkpoints.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
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IF 17.694
Yang Yang,Zhu Xiaojuan,Wang Lili,Lang Junyu,Yao Guohua,Qin Tian,Ren Zhouhong,Chen Liwei,Liu Xi,Li Wei,Wan Ying
Pd catalysts are widely used in alkynol semi-hydrogenation. However, due to the existence of scaling relationships of adsorption energies between the key adsorbed species, the increase in conversion is frequently accompanied by side reactions, thereby reducing the selectivity to alkenols. We report that the simultaneous increase in alkenol selectivity and alkynol conversion is achieved by manipulating interstitial atoms including B, P, C, S and N in Pd catalysts. A negative linear relationship is observed between the activation entropies of 2-methyl-3-butyn-2-ol and 2-methyl-3-buten-2-ol which is highly related to the filling of d -orbital of Pd catalysts by the modification of p -block elements. A catalyst co-modified by B and C atoms has the maximum d charge of Pd that achieves a 17-fold increase in the turn-over frequency values compared to the Lindlar catalysts in the semi-hydrogenation of 2-methyl-3-butyn-2-ol. When the conversion is close to 100%, the selectivity can be as high as 95%.
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INORGANIC CHEMISTRY
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2025
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IF 4.7
Junxiang Lu,Yuting Liu,Shasha Zhang,Juhong Nie,Bing Tang,Jia Guan,Jian Zhang
Regulating the strength of coordination bonds plays an important role in synergizing the activity and stability of single-atom catalysts (SACs) but is often limited due to coordination atoms from the inorganic carrier lattice being tough to modify. It is fascinating yet rarely explored to immobilize organic molecules on lattice atoms for modulating the character of coordination bonds. Herein, a valid inorganic–organic coupling strategy is developed to enhance Pd–O coordination bonds within Pd-SAC for reconciling activity and stability. Nickel hydroxide enriched with Ni2+ vacancies is utilized to bind Pd centers, and dimethylglyoxime (DMG) bonds with its OH groups by H2 reduction, forming a Pd–O-DMG structure. Compared with the pristine Pd–O structure, whose activity descends greatly during the recycling process, the Pd–O-DMG structure makes the activity unchanged after 6 used times for the Suzuki–Miyaura reaction. The Pd-SAC has mild and economic reaction conditions (at 70 °C under air in ethanol without excess base) and good substrate tolerance. Further theoretical calculations show that coupled DMG induces hydrogen bonds on O atoms of the oxazole around Pd centers and thus strengthens Pd–O coordination bonds to exhibit good stability and activity.
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International Journal of Nanomedicine
·
2025
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IF 6.5
Li Gao,Li-Hua Yang,Fang-Cheng Jiang,Wang-Yang Ye,Xin Chen,Zhao-Ji Liu,Rong-Quan He,Wan-Ying Huang,Zhen-Bo Feng,Jin-Liang Kong,Ze-Feng Lai,Gang Chen
Background Although immune checkpoint blocking (ICB) therapeutic agents have significantly improved the survival for many cancer patients, the efficacy of ICB therapy for non-small cell lung cancer (NSCLC) patients remains limited. Combining ICB therapy with other strategies that is able to stimulate tumor immunogenicity or increase infiltration of T cells aroused great concern in cancer therapy.Results Herein, we constructed a kind of AuNP@NH2-PEG-SH/PD-L1 siRNA nanoparticle complex which showed prominent photothermal therapeutic (PTT) effects triggered by NIR laser and could efficiently deliver PD-L1 siRNA into NSCLC cells (knock-down efficiency were 75.8% and 83% in HCC827 and A549 cells). During the process of photothermal stimulation, discrepancies in heat shock protein expression were observed in NSCLC cells. Knocking down PD-L1 expression in NSCLC cells such as A549 and HCC827 cells activated the co-culturing Jurkat cells and enhanced their tumor-killing effect in vitro (cell inhibition rate was 62.65% for HCC827 cells and 57.03% for A549 cells). The gold nanoparticle complexes exhibited remarkable PTT effect for the engrafted NSCLC cells in zebrafish larvas. Furthermore, the nano complexes could promote the activation of the xenografted human peripheral blood mononuclear cells (PBMCs) and enhance the killing of the NSCLC cells in the larvas.Conclusion It is well known that gold nanoparticle is one of the several metal nanoparticles approved for clinical trial by American FDA. This work has demonstrated the outstanding PTT and immunotherapeutic effects of gold nanoparticle complexes on NSCLC, indicating great potential in clinical regiment of lung cancers.
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ChemNanoMat
·
2024
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IF 2.6
Jiangnan Guo,Shuozhen Hu,Xinsheng Zhang,Shigang Sun
Utilizing carbon coated ferroelectric materials to introduce polarization-induced electric field (PIEF) stimulates research of electric field-assisted catalysts for various reactions. However, effect of PIEF on carbon coating mechanism has not been studied. Herein, tourmaline nanoparticles (TNPs) with spontaneous dipole moments were applied as the PIEF supplier and sucrose was utilized as the carbon precursor to synthesize carbon coated TNPs (TNP@SC) to uncover the influence of PIEF on the carbon coating and catalytic activity of Pd toward formic acid decomposition (FAD). PIEF enhanced the adsorption capacity of TNPs for the caramelized intermediate species and increased H+ concentration by facilitating water ionization. Polymerization of adsorbed caramelized intermediate species on TNPs was accelerated. Uniformly coated carbon layer with more defects, larger specific surface area, and higher porosity was coated on TNP. Such surface properties of the carbon layer were beneficial for strongly anchoring ultrafine Pd nanoparticles. Owing to the specific properties of carbon layer and existence of PIEF, Pd/TNP@SC exhibited higher FAD activity than the catalysts absent of PIEF. Stronger PIEF leaded to higher initial turnover frequency. This study provides guidance to supply electric field for catalysis.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Ting Zhang,Yumeng Liu,Qingqing Wu,Lu Zhou,Hongxia Liang,Yi Lu,Mengmeng Dong,Ningning Liu
The detection and discrimination of biothiols are of great significance for tumor cell identification and clinical diagnosis. Recently, nanozymes have been employed to construct biosensor arrays for the determination and differentiation of biothiols. However, most nanozymes currently used are peroxidase-like enzymes, which require highly toxic and unstable hydrogen peroxide (H 2 O 2 ) as a co-substrate to generate reactive oxygen species. Herein, MoS 2 @Pd nanozymes with good Pd dispersion were prepared by in situ growing Pd nanoparticles on MoS 2 nanosheets obtained via liquid-phase exfoliation. This strategy is green, mild, aqueous, and does not require additional reducing agents. Benefiting from the dispersion of Pd active sites and the electronic metal–support interaction, MoS 2 @Pd exhibits superior oxidase catalytic activity, which can effectively trigger the oxidation of the chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) and induce changes in optical absorption. Based on the inhibitory effect of thiols on the chromogenic system, the constructed biosensor can be successfully applied for the sensitive analysis of common thiols. More importantly, the three absorption peaks generated by oxidazed TMB at 370 nm, 450 nm, and 652 nm can serve as three colorimetric channels. Through pattern recognition methods, good differentiation effects can be achieved for biothiols and their mixtures, and successful identification and differentiation of liver cancer cells have been realized. Therefore, MoS 2 @Pd nanozyme provide an easy and cost-effective method, offering new ideas for the construction of sensor arrays and the effective recognition of biothiols and cancer cells.
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