Catalysis Science & Technology
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2025
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IF 4.2
Cheng-Long Li,Rui-Ping Zhang,Lu Hou,Ya-Dong Xie,An-Hui Lu
The selective hydrogenation of alkynols to enols catalyzed by carbon-supported Pd catalysts is a highly attractive reaction for the production of fine chemicals. However, the limited dispersion and stability of Pd species on the carbon support often hindered their catalytic activity. In this study, we developed a “carbon-layer anchored” method to synthesize Pd@NMC monolithic catalysts with tunable Pd exposure by the coating of nitrogen-containing polymer on the wood framework, followed by Pd loading, and carbonization procedures. The exposure of Pd nanoparticles can be controlled through a partial oxidation strategy. As a result, the semi-embedded Pd catalyst (Pd@NMC-250) exhibited superior activity and selectivity (91%) in the semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY). The reaction rate can reach 5110 mol molPd−1 h−1, which is 4.5-fold higher than that of the commercial Lindlar catalyst under identical conditions (308 K, 5 bar H2). Moreover, the monolithic catalyst presented good stability for enduring five cycles. The nitrogen species in the support and the carbon layer deposited on Pd nanoparticles during pyrolysis synergistically promote the Pd anchoring. After mild oxidation, the carbon layer is partially removed to form a semi-embedded Pd@C nanostructure, with the surface exposed and the bottom embedded on the carbon support, which enhances the stability. Furthermore, the monolithic wood-based carbon catalysts are easy to separate from the solution and thus have the potential for operating a variety of liquid-phase catalytic reactions beyond hydrogenation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Mingxin Lv,Liyuan Huai,Guoxin Chen,Xi Zhao,Chunlin Chen,Shenghu Zhou,Jian Zhang
Controlling the selective activation of one or some functional groups as desired is still a challenge in hydrogenation, especially at high substrate concentrations. Herein, Pd-MgO interfaces over Al 2 O 3 were finely regulated for efficiently selective hydrogenation of furan ring in 5-hydroxymethylfurfural (HMF) to produce 5-hydroxymethyltetrahydro-2-furaldehyde (5-HMTHFF) or total hydrogenation to 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF), also inhibiting side reaction. The Pd-MgO/Al 2 O 3 with 12.0 wt% of MgO selectively hydrogenates the furan rings with a 5-HMTHFF yield of 82.4 % while that with 2.0 wt% of MgO totally hydrogenates HMF with a DHMTHF yield of 96.2 % at high substrate concentrations (400 mM). Characterizations and DFT calculations demonstrated that oligomeric MgO species suppress the agglomeration of Pd nanoparticles and strengthen HMF adsorption, consequently promoting total hydrogenation. Furthermore, Pd δ+ -MgO 1-x sites between the crystallized MgO and Pd metal favored tilted adsorption on the interface and weakened the activation of the C O bond, consequently selectively producing 5-HMTHFF.
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AICHE JOURNAL
·
2024
·
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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INTERNATIONAL JOURNAL OF PHARMACEUTICS
·
2024
·
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 Sustainable Chemistry & Engineering
·
2025
·
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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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
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IF 11.2
Nuo Xu,Haoran Zhou,Mingqiang Zhang,Yuchuan Ye,Kaiwen Wang,Yingtang Zhou,Yunfeng Zhu,Yao Zhang
Hydrogen storage plays a pivotal role in the hydrogen industry, yet its current status presents a bottleneck. Diverse strategies have emerged in recent years to address this challenge. MgH 2 has stood out as a promising solid-state hydrogen storage material due to its impressive gravimetric and volumetric hydrogen density, but its practical application is hampered by elevated thermal stability and sluggish kinetics. In this study, we introduce a solution by synthesizing Pd metallene through a one-pot solvothermal method, revealing a distinctive highly curved lamellar structure with a thickness of around 1.6 nm. Incorporating this Pd metallene into MgH 2 results in a composite system wherein the starting dehydrogenation temperature is significantly lowered to 439 K and complete dehydrogenation occurs at 583 K, releasing 6.14 wt.% hydrogen. The activation energy of dehydrogenation for MgH 2 was reduced from 170.4 kJ mol –1 to 79.85 kJ mol –1 after Pd metallene decoration. The enthalpy of dehydrogenation of the MgH 2 –10 wt.% Pd sample was calculated to be 73 kJ mol –1 H 2 –1 and decreased by 4.4 kJ mol –1 H 2 –1 from that of dehydrogenation of pure MgH 2 (77.4 kJ mol –1 H 2 –1 ). Theoretical calculations show that the average formation energy and average adsorption energy of hydrogen vacancies can be significantly reduced in the presence of both Pd clusters and Pd single atoms on the surface of MgH 2 /Mg, respectively. It suggests that the synergistic effect of in situ formed Pd single atoms and clusters significantly improves the hydrogenation and dehydrogenation kinetics. The identified active sites in this study hold potential as references for forthcoming multi-sized active site catalysts, underscoring a significant advancement toward resolving hydrogen storage limitations.
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Science Advances
·
2025
·Vol. 11
·期 32
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IF 12.5
Rui Zhao,Qi Wang,Yancai Yao,Ruizhao Wang,Long Zhao,Zhiwei Hu,Cheng-Wei Kao,Ting-Shan Chan,Wenhuai Li,Qian Zheng,Jiaxian Wang,Xingyue Zou,Kaiyuan Wang,Jie Dai,Xiang-Kui Gu,Lizhi Zhang
Electrochemical hydrogenation (ECH) of unsaturated carbon-heteroatom bonds is essential for chemical transformations but is often limited by a barrier-intensive surface hydrogen transfer process. The interfacial hydrogen bond (HB) network offers a promising pathway for proton transfer but requires addressing the challenge of nondirectional proton shuttling in three-dimensional space. Here, we create hydrophilic CuO x islands on Cu foam (CF) and load electron-enriched Pd (Pd δ− ) single atoms as proton traps (Pd 1 -CuO x /CF) to guide a fast proton transfer along a modified HB network to enhance ECH efficiency. During ECH, hydrophilic CuO x islands dissociate H 2 O into protons and reconstruct the interfacial HB network for facile proton transfer, while the Pd δ− single atoms reorient H 2 O molecules to electrostatically attract and reduce protons to active hydrogen, enabling efficient substrate hydrogenation. With guided proton transfer, Pd 1 -CuO x /CF achieves 99% hydrogenation efficiency for C─Cl bonds, outperforming Pd 1 -CF (69%) and CuO x /CF (57%), and demonstrates high selectivity and Faradaic efficiency in hydrogenating C═O and C≡N bonds to produce valuable chemicals.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Jia Yao,Pengtao Chen,Dingqi Xie,Jianqingchen Chen,Xiao Lin,Yujin Xu
Radiotherapy (RT) is a widely used clinical treatment for cancer, leveraging ionizing radiation; however, some patients exhibit resistance to radiation due to insufficient reactive oxygen species (ROS) production. Copper-based nanomaterials represent a promising class of antitumor agents capable of generating abundant ROS. In this study, R837 and Cu2–xSe were incorporated into PLGA (50:50)20k-PEG2k-iRGD to develop a targeted nanomaterial for tumor therapy. These nanoparticles effectively induced cuproptosis, inhibited tumor cell proliferation, remodeled the tumor immune microenvironment (TME), and promoted immunogenic cell death (ICD), thereby enhancing the efficacy of PD-1 checkpoint blockade therapy (αPD-1). Furthermore, our results demonstrated that the Cu2–xSe(R837)-iRGD nanoformulations, in combination with radiotherapy, promoted the infiltration of CD8+ T cells and activated antitumor immune responses in vivo. In conclusion, our study confirmed that Cu2–xSe(R837)-iRGD nanoformulations combined with radiotherapy yielded promising therapeutic outcomes and held potential for clinical application in osteosarcoma (OS) treatment.
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Advanced Sensor Research
·
2025
·
IF 3.5
Jiahong Wen,Yaxin Wang,Ruoning Chu,Jinhai Li,Ze Chen,Yongjun Zhang,Xiaoyu Zhao,Qi-Qi Fu
Freon refrigerants, whose leakage will cause serious safety and environmental issues, have an urgent need of developing leakage detection technologies. Conventional metal oxide semiconductor (MOS) gas sensors exhibit limited efficacy in detecting halogenated Freons due to their chemical inertness and weak charge-transfer interactions. While recent innovations employing mesoporous γ-Al 2 O 3 overlayers have enabled Freon detection via catalytic decomposition sensing mechanism, the achieved sensing performance remains suboptimal. In this work, this issue is addressed by engineering a Pd-doped mesoporous γ-Al 2 O 3 /SnO 2 (Pd-γ-Al 2 O 3 /SnO 2 ) gas sensor. The doped Pd atoms not only accelerate the decomposition of Freon molecules on the catalytic layer but also induce the Schottky-barrier effect in the SnO 2 sensing layer. Benefiting from the synergistic effect, the Pd-γ-Al 2 O 3 /SnO 2 gas sensor shows outstanding response, good stability, repeatability, selectivity, and rarely-reported universality in sensing different Freon gases. Notably, a valuable solution is demonstrated in the leakage detection of next-generation refrigerants, Freon R1234yf. The sensing mechanism is deduced by exhaust gas components identification. These results highlight the promising potential for addressing the real-world needs of Freon refrigerant leakage detection technology.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
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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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Ruichun Nan,Xinxin Zhang,Yuheng Zhao,Hongda Huang,Yapeng Niu,Ying Yan,Litao Zhang,Bingkun Liu,Jingtao Zhang,Xianzhong Yin
Herein, Pd-doped CeO 2 was synthesized by facile hydrothermal methods, X-ray diffraction (XRD) analysis and transmission electron microscope (TEM) suggests that Pd is successfully incorporated into the CeO 2 lattice. X-ray photoelectron spectroscopy (XPS), UV–Vis and PL demonstrated that Pd-doped CeO 2 improve the light absorption and enhance the electron-hole separation of CeO 2 . The prepared Pd-CeO 2 exhibits outstanding bactericidal performance. Specifically, 1 % Pd-CeO 2 can completely inactivate Ralstonia solanacearum with an initial concentration of 2 × 10 7 CFU/mL within 60 min, while also demonstrating effective killing against Escherichia coli and various pathogenic fungi. EPR demonstrated that Pd doping into CeO 2 could increase the number of vacancies, electron spin resonance (ESR) tests demonstrated that e - play a major role in the photocatalytic process, disruption of the cellular structure of E. coli during photocatalytic treatment as evidenced by scanning electron microscopy (SEM) tests. Promising reference for the practical application of precious metal photo catalysts in disinfection.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
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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