International Journal of Electrochemical Science
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2023
·
IF 1.5
Jing Leng,Ping Li,Ling Bai,Yingqiong Peng,Yongfang Yu,Limin Lu
A Pd nanoparticles-graphene oxide (PdNPs/GO) hybrid as a highly sensitive sensing platform for determination of rutin was successfully prepared by a facile one-pot redox synthesis approach. Formation of PdNPs and loading onto the GO nanosheets were accomplished simultaneously by a redox reaction between H2PdCl4 and GO, without use of any additional reductants. Scanning electron microscopy (SEM) results demonstrated that PdNPs with an average size of 60 nm were distributed on the surface of GO nanosheets. Compared with the GO modified electrode, the PdNPs/GO modified electrode showed a better electrocatalytic activity toward the oxidation of rutin with larger peak current. Then the PdNPs/GO hybrid can be used as an enhanced sensing platform for the electrochemical determination of rutin. Under the optimal conditions, the anodic peak current was linear to the concentration of rutin in the range from 0.005 to 6 μM with the detection limit of 0.001 μM (S/N = 3). More importantly, the developed sensor can be used for the determination of rutin in medicine tablets with satisfactory results.
研究领域:
材料科学
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分析化学
·
药物分析
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Wenhui Zou,Yingcen Liu,Caicheng Song,Hua Lin,He Huang,Wanyue Ye,Rongwen Lu,Shufen Zhang
A series of PdO@MCM-41-x was in situ synthesized by a facile one-pot method, and their catalytic performance for dehydrogenation of formic acid was investigated. The PdO nanoparticles were immobilized in MCM-41 channel with small size of 2.2–2.5 nm due to the confinement of mesoporous silica . The initial turnover frequency (TOF) of as-prepared catalyst can reach 1096 h −1 at 323 K with 100% hydrogen selectivity. The hydrogen production activity was better than that of catalyst priorly reduced by hydrogen because of the gradual reduction of PdO nanoparticles and generation of fresh Pd(0) during the formic acid dehydrogenation process, which was confirmed by XPS characterization and catalytic system monitoring. It provides a new way for the preparation of simple and efficient catalysts for hydrogen production , which has great application potential.
研究领域:
化学
·
催化材料科学
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Cell Reports Medicine
·
2026
·
IF 14
Qiang Zhang,Yue Kong,Yinglin Long,Xue Li,Liang Wang,Zhanhao Luo,Xiaoya Yang,Yanchun Xie,Quanwei Yu,Jing Yu,Dayi Liang,Wenhao Yuan,Xiaomin Cheng,Yaqi Su,Kaisa Cui,Guobao Tian,Zhen He,Ping Lan
Immune evasion remains a major challenge in colorectal cancer (CRC) treatment. Here, we identify that druggable β-catenin palmitoylation at cysteine 466 (C466) by ZDHHC5 acts as a competitive switch, displacing S-nitrosylation and coordinating an immunosuppressive program. The palmitoylated state stabilizes the β-catenin/TCF4 complex, which simultaneously upregulates SLC7A11 to suppress immunogenic ferroptosis, critical for CD8 + T cell priming, and PD-L1 to inhibit cytotoxic CD8 + T cells, thereby impairing both the initiation and effector phases of anti-tumor immunity. Clinically, ZDHHC5 expression predicts poor survival and resistance to anti-PD-L1 therapy. Silencing ZDHHC5 reduced tumor growth in patient-derived organoids and xenografts, while Zdhhc5 ablation in mice inhibited CRC progression by reversing immunogenic ferroptosis suppression and alleviating PD-L1-mediated T cell inhibition. Importantly, β-cat-oxazole, a first-in-class inhibitor, disrupts ZDHHC5-β-catenin binding, thereby restoring immunogenic ferroptosis and blocking PD-L1-mediated immunosuppression, ultimately suppressing tumor growth. Our findings establish targeting of this palmitoyl-switch as a precision strategy to overcome therapeutic resistance.
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LANGMUIR
·
2026
·
IF 3.9
Sha Yang,Minghui Wang,Hao Li,Changmin Li,Yaomei Long,Qinglai Yang,Xiaofeng Tan
Antimicrobial resistance has become a pivotal global public health concern, significantly moderating the effectiveness of antibiotic therapies. Metallic hydrogels, as a highly representative nanozyme, have shown promise in combating drug-resistant bacterial infections. Herein, we develop an innovative AuCu@Pd hydrogel nanozyme utilizing a facile water/ethanol-phase method, achieving gelation within 40 min. The building blocks of AuCu@Pd hydrogels exhibit dendritic and core–shell structures, facilitated by the regulation of nanowire-like morphologies through galvanic replacement and ascorbic acid induction effects. The AuCu@Pd hydrogels demonstrate peroxidase-like (POD-like) and oxidase-like (OD-like) activities, facilitating the conversion of H2O2 and O2 into highly cytotoxic reactive oxygen species (ROS) to disrupt bacterial cell structures. Moreover, the AuCu@Pd hydrogels modulate the infectious microenvironment by depleting glutathione (GSH), thereby promoting the production of reactive oxygen species (ROS) and enhancing their bactericidal effects against methicillin-resistant Staphylococcus aureus (MRSA) and Escherichia coli (E. coli). Notably, AuCu@Pd hydrogels demonstrate a high photothermal conversion efficiency (η) of 61.1% and superior photothermal stability, significantly boosting the multienzyme-like activity for efficient antibacterial therapy. In addition, these hydrogels exhibit excellent biocompatibility in vivo and significantly accelerate MRSA-infected skin wound healing. This work offers novel insights into the design of highly efficient metallic hydrogels and proposes an effective strategy for the synergistic treatment of MRSA infections for biomedical applications.
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ChemNanoMat
·
2026
·Vol. 12
·期 3
·e202500634
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IF 2.6
Jie Gao,Yan Wu,Guozheng Lv,Mengyang Li,Wei Tian,Na Du,Zhichao Zhang,Shuang Han,Feng Cao
High-entropy alloys (HEAs), composed of multiple principal elements in near-equiatomic ratios, offer vast compositional tunability and synergistic electronic interactions for heterogeneous catalysis. Here, we report a nitrogen-doped carbon nanofiber (N–CNF) encapsulated HEA catalyst, Fe 26 Co 13 Ni 24 Cr 10 Cu 17 Pd 10 @N–CNFs, synthesized via electrospinning followed by controlled thermal treatment. The resulting ~16 nm HEA nanoparticles are uniformly embedded within a conductive N-doped carbon matrix, forming a robust core–shell architecture. Despite the low Pd loading (10 at%), the catalyst achieves 99% nitrobenzene conversion with >99% aniline selectivity at 60°C—an 8.9-fold activity enhancement over Pd@N–CNFs. Furthermore, it retains >95% conversion after five consecutive reaction cycles, underscoring its excellent structural and catalytic durability. The outstanding performance arises from Pd-induced electronic modulation within the entropy-stabilized multimetallic matrix and synergistic confinement by the N-doped carbon framework. This work establishes a cost-efficient and durable HEA-based platform for selective hydrogenation, offering new insights into entropy-driven electronic regulation in multimetallic catalysts.
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Theranostics
·
2026
·Vol. 16
·期 8
·4128
·
IF 13.3
Yuhan Mai,Yanling Chen,Chao Li,Tongyao Wang,Shangli Ding,Hao Zhang,Haili Lin,Longguang Jiang,Cai Yuan,Xiaolei Zhou,Mingdong Huang,Peng Xu
Background: Compared to the lymphodepleting chemotherapy and radiotherapy, photodynamic therapy (PDT) is an oncotherapeutic modality inherently stimulating immune responses by inducing immunogenic cell death (ICD). However, the immunosuppressive tumor microenvironment (TME) frequently attenuates PDT-elicited immune responses, limiting its efficacy in eradicating distant and metastatic tumor cells. Methods: To maximize the immunotherapeutic efficacy of PDT, we developed a photodynamic immunotherapeutic liposomal nanoplatform (PDIT-liposome) integrating components targeting sequential stages of the antitumor immune response: 1) a phthalocyanine photosensitizer to induce ICD, 2) a factor Xa inhibitor (rivaroxaban) to promote T-cell priming, 3) and a program death-ligand 1 inhibitor to augment cytotoxic T lymphocyte (CTL) attack. To enable light-controlled drug release at tumor sites, the liposome was constructed with reactive oxygen species-sensitive phospholipids in response to the PDT effect. Results : PDIT-liposomes were characterized via multiple physicochemical and optical evaluations. Comprehensive in vitro and in vivo investigations confirmed that PDIT-liposomes significantly enhanced antitumor efficacy compared to monotherapies and dual combinations. In a subcutaneous implantation tumor model, PDIT-liposome achieved a 91.7% antitumor rate compared to 21.83% (P-liposome), 46.78% (PD-liposome), and 51.08% (PR-liposome) (p < 0.001). Mechanistic analysis revealed enhanced dendritic cell maturation (8-fold increase in CD11c + cells) and T-cell priming (2.3-fold increase in CD8 + T cells) in tumor-draining lymph nodes (TDLNs), and CTL-mediated cytotoxicity (5.4-fold increase in CD107a + activated CTLs) in TME. Notably, PDIT therapy induced long-term immunological memory, which suppressed 90.68% tumor reoccurrence and metastasis. Conclusion: This study presents a strategy to amplify PDT-elicited immunotherapeutic efficacy by synergizing agents targeting distinct stages of the immune response. It also theoretically validates the synergy of PDT, anticoagulation therapy, and immune checkpoint inhibition in cancer treatment.
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RARE METALS
·
2023
·Vol. 42
·期 5
·1516-1525
·
IF 8.8
Wang Mei-Ling,Zhao Jin,Wang Jin-Jin,Zhang Jun-Ming,Tian Yu-Zhu,Yue Zhi-Zhu,Li Dong,Hu Tian-Jun,Jia Jian-Feng,Wu Hai-Shun
metal oxide electronic interactions in composite electrocatalysts have a considerable impact on their catalytic capability. In this study, we successfully synthesized an electrocatalytic material composed of MoO 3 /C species-supported Pd nanoparticles (Pd-MoO 3 /C) using a convenient hydrothermal method, which exhibited excellent catalytic activities for both ethanol oxidation and oxygen reduction in KOH media. The specific activity of Pd-MoO 3 /C toward ethanol oxidation with MoO 3 loading (40 wt%) was ~ 2.6 times greater than that for the commercial Pd/C (10 wt%) with the same Pd content. In particular, the activity could effectively hold up to ~ 60% of its maximum activity after 500-cycle tests, demonstrating improved cyclical stability. Notably, the fast electron transfer kinetics toward oxygen reduction for Pd-MoO 3 /C (40%) were also comparable to those of commercial Pt/C (20 wt%) catalysts. These superior electrochemical features are primarily derived from the stronger electronic coupling between Pd and MoO 3 through charge transfer, which can supply more active centers and improve the anti-poisoning ability. Meanwhile, the MoO 3 species in the Pd-MoO 3 /C composite may provide additional benefits in terms of electrical conductivity and dispersion. Graphical Abstract
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Xiao-Chao Chen,Tian Lan,Jian Zhu,Sibin Ying,Guang-Hui Shi,Kai-Chun Zhao,Lin Guo,Yong Lu,Ye Liu
The tripodal phosphine [ L1 , 1,1,1-tris(diphenylphosphino-methyl)ethane] was applied to control the activity, regioselectivity, and stability of the involved Pd-catalyst in anti-Markovnikov hydroaminocarbonylation of alkenes with aromatic amines for the synthesis of linear-amides. Due to the unique characters of L1 in terms of the steric bulkiness, the switching-coordination mode from tripodal phosphine to bidental one, and the robustness against moisture and oxygen, L1 conferred to Pd-catalyst with the high activity, good regioselectivity, and excellent stability for this carbonylation, leading to 44 ∼ 87 % yields of the target amides with L/B of greater than 80/20. The in situ high-pressure FT-IR analysis and the DFT calculations verified that L1 not only promoted the formation and stability of Pd II -H active species (ν ca. 1932 cm −1 ) but also facilitated the anti-Markovnikov’s addition of alkenes with Pd II -H bond due to the favorable energy level of linear intermediate ( B-1 ). In addition, since L1 can coordinate to Pd(II)-center as a bidental chelator as fulfill catalysis and then coordinate to Pd(0)-center as an tripodal pincer, Pd-catalyst was protected timely by L1 against metal-deposition (Pd 0 -black precipitation) to guarantee its stability for recycling uses for 5 runs without activity loss.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Jun Li,Liying Cai,Xiaosi Liang,Shuke Huang,Xiaosha Wang,Yongshuai Kang,Yongjian Zhao,Lei Zhang,Chenyang Zhao
Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect. Herein, an innovative method was developed to synthesize C-doped Pd interstitial nanoalloy using palladium acetate both as metal precursor and C dopant. Elaborate characterizations demonstrated that C atoms were successfully doped into the Pd lattice via self-catalytic decomposition of acetate ions. The as-synthesized C-doped Pd catalysts showed excellent activity and durable stability for formic acid electrooxidation. The mass activity and specific activity at 0.6 V of C-doped Pd were approximately 2.59 A/mg and 3.50 mA cm −2 , i.e., 2.4 and 2.6 times of Pd, respectively. DFT calculations revealed that interstitial doping with C atoms induced differentiation of Pd sites. The strong noncovalent interaction between the Pd sites and the key intermediates endowed Pd with high-selectivity to direct routes and enhanced CO tolerance. This work presents a sites-differentiation strategy for metallic catalysts to improve the electrocatalysis.
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ENERGY
·
2022
·
IF 8.857
Heping Xie,Hailong Liao,Shuo Zhai,Tao Liu,Yifan Wu,Fuhuan Wang,Junbiao Li,Yuan Zhang,Bin Chen
Using aqueous Zn–CO 2 batteries to store renewable energy and produce valuable chemicals using CO 2 as the source is a promising method for CO 2 mitigation, that is alternative to traditional energy-costing CO 2 capture/storage technologies. However, the lack of efficient CO 2 -reduction catalysts significantly hinders the efficiency of such batteries. In this study, an efficient perovskite cathode, Pd-doped La 2 CuO 4 , was successfully developed for the cathodic CO 2 reduction reaction (CO 2 RR), and the optimal doping ratio of La 2 Cu 1-x Pd x O 4 ( x = 0.05) was determined. Compared with the pristine La 2 CuO 4 catalyst, the current density for the CO 2 RR in the H-cell and the Faraday efficiency of CO production are both increased by ∼50% when operated −1.0 V (vs RHE). As a result, the peak power density of a Zn–CO 2 battery using the Pd-doped La 2 CuO 4 catalyst reached 0.75 mW cm −2 at 2.23 mA cm −2 by an enhancement ratio of 25%. Density functional theory calculations revealed that the *CO desorption processes on the cathode were enhanced owing to Pd doping, which accounted for the enhanced CO 2 RR activity and selectivity. The findings of this study show the potential application of perovskite catalysts in the cathode of Zn–CO 2 batteries and provide an effective method for battery performance enhancement via the facile Pd doping.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 2
·1-10
·
IF 6.408
Huang Hui,Xie Shuqian,Deng Lu,Yuan Jie,Yue Ruirui,Xu Jingkun
A nanocomposite of rGO/MXene-Pd/rGO with hierarchical structure based on Ti 3 C 2 T x MXene, Pd nanoparticles, and reduced graphene oxide (rGO) was synthesized by a green approach. Ti 3 C 2 T x MXene decorated with Pd nanoparticles (MXene-Pd) was prepared first. Then, graphene oxide (GO), MXene-Pd, and GO were coated on the surface of the glassy carbon electrode (GCE) in sequence. After each coating of the GO layer, the GO nanosheets were reduced to rGO electrochemically. The fabricated rGO/MXene-Pd/rGO hierarchical framework performs a pie structure with MXene-Pd as the stuffing and rGO nanosheets as the crust, which will be beneficial to the enhancement of its electrochemical sensing performance. As compared with other electrodes, the rGO/MXene-Pd/rGO/GCE exhibited higher electrocatalytic activity and better sensing performance for luteolin detection, with a wide linear range of 6.0 × 10 −10 to 8 × 10 −7 M and 1.0 × 10 −6 to 1.0 × 10 −5 M (oxidation peak potential E pa = 0.34 V vs . SCE), a low detection limit of 2.0 × 10 −10 M, and a high sensitivity of 112.72 µA µM −1 cm −2 . Moreover, the fabricated sensor also showed high selectivity, reproducibility, and repeatability toward the detection of luteolin. The real sample analysis for luteolin in honeysuckle was successfully carried out by rGO/MXene-Pd/rGO and verified with high-performance liquid chromatography (HPLC) analysis techniques with acceptable results. All the above tests indicate the promising application prospect of the rGO/MXene-Pd/rGO framework for luteolin detection in honeysuckle and other herbs containing luteolin. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zongtang Liu,Haini Yang,Mian Wang,Yufeng Sun,Zhenghao Fei,Shujuan Chen,Rui Luo,Lin Hu,Chenggang Gu
Effective removal of polybrominated diphenyl ethers (PBDEs) from the environment is essential for the ecosystem and human health. Reductive debromination of PBDEs by nanoscale zerovalent iron (nZVI) has become an important technology. However, the agglomeration and low persistence catalytic activity of nZVI particles have become urgent problems to be improved. Herein, we report the first application of a new organo-attapulgite (OA) supported Fe/Pd nanoparticles (OA-Fe/Pd) composite for decabromodiphenyl ether (BDE209) removal. BDE209 was efficiently removed using OA-Fe/Pd with a reaction rate that was 9.97 times greater than that of the nZVI due to the synergetic effect of support material OA and Pd loading. OA could prevent nZVI particles from agglomeration and adsorb BDE209 molecules to its surface. Pd could supply atomic hydrogen and also prevent the oxidation of nZVI particles. The degradation of BDE209 by OA-Fe/Pd was affected by many factors and followed pseudo first-order kinetics. The degradation of BDE209 by OA-Fe/Pd underwent a stepwise debromination manner with the H-transfer dominant mechanism. BDE209 (25 mg∙L -1 ) could be degraded to penta-BDEs to diphenyl ether (DE) by 3.0 g∙L -1 OA-Fe/Pd within 240 min under neutral condition. This study provides some inspiration for improving the removal efficiency of PBDEs with nZVI-based materials.
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