INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Zhuhao Li,Fei Yuan,Tianyun Cui,Changhai Liang,Chuang Li
At present, most of the catalysts used for heterogeneous hydrogenation of nitrile butadiene rubber (NBR) are noble metal catalysts, which require high metal loading but low metal utilization and face challenges in recovery, leading to significant resource waste. The steric hindrance imposed by the large polymer molecules renders the hydrogenation of unsaturated C═C bonds in the backbone particularly challenging, and the degree of hydrogenation is low. In this experiment, Pd–Ni bimetallic nanocatalyst was prepared by co-impregnation method. The catalyst has uniformly distributed catalytic site and high selectivity for C═C bond hydrogenation and achieved a hydrogenation degree of 96% under optimized reaction conditions. The electronic state of Pd is modulated by Ni, enhancing hydrogen activation and catalytic activity. This study provides a novel strategy for developing NBR hydrogenation catalysts, which is significant for the large-scale production of high-value-added HNBR.
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AICHE JOURNAL
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2024
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IF 3.5
Bin Zhang,Chen Yang,Yunjiao Jia,Guohui Nie,Guidong Yang
Nitrate reduction toward ammonia is pivotal in energy and environmental domains but faces challenges in achieving simultaneous high selectivity and activity. Manipulating interactions between intermediates and metal species is deemed effective for catalytic enhancement. In this study, a uniformly configured Fe 1 -N 4 single-atom catalyst with four-coordination was synthesized. Subsequent deposition of thiol-poisoned Pd nanoclusters provided a platform to investigate the neighboring effect of Pd nanoclusters, excluding activity influences from Pd catalysts. Through this neighbor engineering, the Fe 3d electron spin configuration shifted from low spin to medium spin (MS). Experimental and theoretical analyses affirmed that MS Fe species optimized nitrate reduction by enhancing the *NO desorption process. This spin-modulated Fe single-atom catalyst demonstrated superior activity (392.16 mmol −1 g cat −1 h −1 , ~40 mol −1 g Fe −1 h −1 ) and a Faraday efficiency of 98.6% at −0.5 V vs. RHE, surpassing reported values. This study presents a promising strategy for nitrogen-chemistry transition metal catalysts.
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ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Yan Shao,Jun Wan,Xiaoxia Ou,Cui Quan,Ningbo Gao,Xin Wang,Feng Zeng,Rongsheng Cai,Xiaolei Fan,Huanhao Chen
Engineering Pd–In2O3 interaction is key to developing catalysts with the desired CO2 hydrogenation activity toward methanol synthesis. Here, the crystalline phase of In2O3 nanospheres was tuned by changing the calcination temperature, which was found to affect the Pd–In2O3 interaction and thus the supported Pd states and CO2 hydrogenation performance of the prepared Pd/In2O3-a catalysts (where a refers to the calcination temperature for preparing In2O3). The fresh Pd/In2O3-a catalysts show varied initial activities, and after the induction period, their performance stabilized though being different. During the 100 h catalysis, catalyst microstructures changed, showing Pd aggregation and Pd–In alloying, which was related to the nature of the crystalline phase of In2O3. The hexagonal (h-In2O3) phase in Pd/In2O3-400 possesses concentrated surface OH groups and limited mobility. The relatively poor mobility limits Pd–In alloying, which possibly suppresses the hydrogen spillover effect, causing low CO2 conversion (8%) and methanol selectivity (45%) under steady-state conditions at 5 MPa and 300 °C. Conversely, the cubic In2O3 (c-In2O3) phase promotes Pd–In alloying and modifies Pd–In2O3 interaction during the reaction. The activity data show that Pd/In2O3-600 with the mixed phases of In2O3 (h/c-In2O3) demonstrated appropriate Pd–In2O3 interaction, leading to the Pd core InOx shell structure with the comparatively best methanol selectivity of about 65% at steady state. Conversely, Pd/In2O3-800 with the pure cubic In2O3 (c-In2O3) phase and a relatively low specific surface area of 16 m2 g–1 encourages the sintering of Pd and thereby the formation of homogeneous Pd–In alloys, having a moderate methanol selectivity of about 50%. These findings highlight the importance of the In2O3 crystal phase engineering in the catalytic CO2 hydrogenation over Pd/In2O3 catalysts and the dynamics of Pd–In interactions, which affect the methanol yield.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2024
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IF 5.3
Renjiang Kong,Jiaqi Huang,Yeyang Wu,Ni Yan,Xin Chen,Hong Cheng
The unsatisfactory immunotherapeutic responses are primarily attributed to the insufficient immune recognition and the presence of an immunosuppressive tumor microenvironment (ITM). This study focuses on the development of a tricomponent immunoactivating nanomedicine called TIN that combines a photosensitizer, an inhibitor of epidermal growth factor receptor (EGFR) and a CSF-1R inhibitor to enable photodynamic immunotherapy by downregulating PD-L1 expression and repolarizing tumor-associated macrophages (TAMs). TIN is designed to facilitate the drug delivery and target specific pathways involved in tumor progression. By inhibiting the activity of EGFR and CSF-1R, TIN reduces PD-L1 expression on tumor cells and induces the TAMs polarization to M1 phenotype, restoring the immune recognition of T cells and the phagocytosis of macrophage to reshape the immunosuppressive microenvironment. Additionally, the photodynamic therapy (PDT) of TIN can greatly destroy the primary tumor and trigger immunogenic cell death (ICD). Importantly, the immune checkpoint blockade effect of TIN can enhance the immune response of PDT-induced ICD for metastatic tumor treatment. This study presents a self-assembling strategy for the development of an all-in-one nanomedicine, effectively integrating multiple therapeutic modalities to provide a comprehensive and systemic approach for tumor suppression.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Xin Huang,Jiawei Zhu,Chuhuang Dong,Yuqing Li,Qing Yu,Xuan Wang,Zhejie Chen,Jiabei Li,Yu Yang,Haifang Wang
Ag2S quantum dots (QDs) show superior optical properties in the NIR-II region and display significant clinical potential with favorable biocompatibility. However, inherent defects of low targeting and poor solubility necessitate practical modification methods to achieve the theranostics of Ag2S QDs. Herein, we used rolling circle amplification (RCA) techniques to obtain long single-stranded DNA containing the PD-L1 aptamer and C-rich DNA palindromic sequence. The C-rich DNA palindromic sequences can specifically chelate Ag2+ and thus serve as a template to result in biomimetic mineralization and formation of pApt-Ag2S QDs. These QDs enable specific targeting and illuminate hot tumors with high PD-L1 expression effectively, serving as excellent molecular targeted probes. In addition, due to the high NIR-II absorption of Ag2S QDs, pApt-Ag2S QDs exhibit remarkable photothermal properties. And besides, polyvalent PD-L1 aptamers can recognize PD-L1 protein and effectively block the inhibitory signal of PD-L1 on T cells, enabling efficient theranostics through the synergistic effect of photothermal therapy and immune checkpoint blocking therapy. Summary, we enhance the biological stability and antibleaching ability of Ag2S QDs using long single-stranded DNA as a template, thereby establishing a theranostic platform that specifically targets PD-L1 high-expressing inflamed tumors and demonstrates excellent performance both in vitro and in vivo.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Jiaoyang Wang,Qingtao Zeng,Kaile Cao,Yanshuai Cui,Haiyan Xiao,Longgang Wang
Organophosphorus pesticides (OPs) pose a significant threat to food safety due to their high toxicity and tendency to bioaccumulate. Conventional detection methods are constrained by reliance on specialized equipment and complex procedures, hindering rapid, on-site screening. In this study, a green synthesis approach was employed using hawthorn polysaccharide (HP) as a natural stabilizer to fabricate bimetallic Pd@Ru nanozymes (HP-Pd m Ru n NPs). The synergistic effect between palladium and ruthenium markedly enhanced the nanozymes' peroxidase-like catalytic activity and stability. Their catalytic behavior followed typical Michaelis–Menten kinetics, exhibiting a strong affinity for the substrate 3,3′,5,5′-tetramethylbenzidine (TMB). A colorimetric biosensor based on HP-Pd 10 Ru 20 NPs enabled rapid and sensitive detection of glyphosate, with a detection limit as low as 0.179 ng/mL and a linear range of 0.0002–200 μg/mL. The biosensor demonstrated excellent selectivity and recovery, offering promising potential for bioanalytical applications and contributing to the development of environmentally friendly, cost-effective technologies for detecting OPs residues.
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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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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2025
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IF 6.2
Wanchen Zhu,Zhongyang Luo,Feiting Miao,Longyi Liu
Biomass hydropyrolysis vapor upgrading (HPVU) is a promising approach for biofuel production, where metallic catalysts play a key role in oxygen removal and aromatic hydrocarbon formation. In this study, Pd/HZSM-5 and Mo/γAl 2 O 3 catalysts were prepared and utilized individually or in combination to investigate their effects on poplar HPVU in a continuous-flow reactor. Meanwhile, the influence of upgrading temperature on hydrodeoxygenation (HDO) reactions was studied. At an upgrading temperature of 400 ℃, combination of Pd/HZSM-5 and Mo/γAl₂O₃ resulted in an organic phase yield of 9.19 wt%. The mass yield and selectivity of aromatic hydrocarbons reached 8.13 wt% and 93.4 %, respectively, with selectivity of C8 + monocyclic aromatic hydrocarbons accounting for 56.7 %. The overall mass balance was 96.2 %. The presence of Pd promotes hydrogenation and hydroalkylation reactions, while Mo/γAl₂O₃ enhances deoxygenation. Additionally, its mesoporous structure facilitates reactant diffusion. The density functional theory calculations confirmed that Pd could efficiently activate H 2 and thus provide hydrogen radicals for HDO on Mo/γAl₂O₃ surface, which revealed the synergistic effect of these two catalysts. This study highlights that noble-metal catalyst aided by oxophilic metal catalyst can make a significant contribution to biomass HPVU.
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JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Wenxing Jiang,Qiqi Wan,Endao Zhang,Yingying Liu,Junbo Hou,Min Yang,Xiaodong Zhuang,Changchun Ke
This study presents a novel direct methylhydrazine fuel cell (DMHFC) utilizing a hydrothermally synthesized Pd-Ni(OH) 2 composite catalyst supported on nickel foam (Pd-Ni(OH) 2 /NF) as the anode. The Pd-Ni(OH) 2 /NF features a three-dimensional hierarchical architecture with dispersed Pd nanoparticles (0.08 mg cm −2 ) chemically anchored via Pd-O-Ni bonds in the Ni(OH) 2 nanosheet matrix, as confirmed by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS) analyses. The electrode demonstrates superior electrocatalytic activity for the methylhydrazine oxidation reaction (MHOR), attributed to enhanced active site accessibility, charge transfer efficiency, and optimized mass transport. Differential electrochemical mass spectrometry (DEMS) reveals complete oxidation of hydrazine fragments to N 2 with suppressed NH 3 byproduct formation relative to Pd/C. Systematic optimization of operating conditions yields a peak power density of 30.5 mW cm −2 (oxygen as the oxidant, 80 °C) and 110 mW cm −2 (hydrogen peroxide as the oxidant, 80 °C), with performance trade-offs observed between reaction kinetics and fuel crossover. This work validates the feasibility of DMHFC technology, highlighting the potential of methylhydrazine as a high-energy-density fuel for portable systems, while providing insights into electrode design and performance optimization for advanced energy conversion devices.
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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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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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Nature Communications
·
2022
·Vol. 13
·期 1
·1-17
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IF 17.694
Guan Xin,Sun Liping,Shen Yuting,Jin Fengshan,Bo Xiaowan,Zhu Chunyan,Han Xiaoxia,Li Xiaolong,Chen Yu,Xu Huixiong,Yue Wenwen
Cancer recurrence after surgical resection (SR) is a considerable challenge, and the biological effect of SR on the tumor microenvironment (TME) that is pivotal in determining postsurgical treatment efficacy remains poorly understood. Here, with an experimental model, we demonstrate that the genomic landscape shaped by SR creates an immunosuppressive milieu characterized by hypoxia and high-influx of myeloid cells, fostering cancer progression and hindering PD-L1 blockade therapy. To address this issue, we engineer a radio-immunostimulant nanomedicine (IPI549@HMP) capable of targeting myeloid cells, and catalyzing endogenous H 2 O 2 into O 2 to achieve hypoxia-relieved radiotherapy (RT). The enhanced RT-mediated immunogenic effect results in postsurgical TME reprogramming and increased susceptibility to anti-PD-L1 therapy, which can suppress/eradicate locally residual and distant tumors, and elicits strong immune memory effects to resist tumor rechallenge. Our radioimmunotherapy points to a simple and effective therapeutic intervention against postsurgical cancer recurrence and metastasis.
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