MICROCHEMICAL JOURNAL
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2025
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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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ChemNanoMat
·
2024
·
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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
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IF 3.9
Bin Zhang,Xiaodong Guo,Xin Feng,Xiaoxia Duan,Guilong Wang,Chao Yang
The debenzylation reaction of hexabenzylhexaazaisowurtzitane (HBIW) and 2,6,8,12-tetraacetyl-4,10-dibenzyl-2,4,6,8,10,12-hexaazaisowurtzitane (TADBIW) to synthesize 2,6,8,12-tetraacetyl-2,4,6,8,10,12-hexaazaisowurtzitane (TAIW) is the major challenge in the production of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (HNIW). This is primarily attributed to the reaction needing a lot of palladium catalysts, which tend to deactivate rapidly during the process. In this work, a series of Pd(OH)2/C catalysts were successfully prepared through a convenient deposition-precipitation method by controlling the flow rate of the PdCl2 solution. Employing the 10% Pd(OH)2/C–F0.5 sample, the debenzylation reaction was successfully completed with a lower usage of Pd and shorter time of reaction. For the HBIW debenzylation reaction, the yield of TADBIW was 87.4% at low temperature (25 °C) when 1‰ Pd/HBIW was used, and the higher yield was 89.8% at high temperature (45 °C) when 3‰ Pd/HBIW was used. The TADBIW/Pd/h values of them were 42.5 and 95.7, respectively. For the TADBIW debenzylation reaction, the complete conversion of the reactant was realized when Pd/TADBIW was 2‰. The value of TAIW/Pd/h was 154.6 when Pd/TADBIW was 4‰, which was higher than the reports. Compared to the reported catalysts, the dosage of Pd used in the debenzylation reactions of HBIW and TADBIW was significantly decreased. Furthermore, the 10% Pd(OH)2/C–F0.5 sample was recycled six times with similar performance, demonstrating excellent stability. Based on the analysis of characterization results, it is effortless to find that the flow rate of the PdCl2 solution plays a key role in controlling the adsorption behavior of palladium species on activated carbon. The lower flow rate is beneficial to obtaining Pd nanoparticles with a smaller size, a higher proportion of Pd2+, and a higher metal distribution. This study may provide a simple way to develop palladium catalysts with high performance for related applications.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Yixin Xu,Yiping Wang,Ying Li,Na Su,Shuozhen Hu,Xinsheng Zhang
Direct formic acid fuel cells (DFAFCs) are promising portable power sources with the advantages of easy handling and high theoretical open-circuit voltage. Exploring efficient Pd-based catalysts for formic acid oxidation (FAO) on the anode is important for the widespread use of DFAFCs. However, formic acid decomposition on the Pd surface restricts the FAO activity of the catalyst, in which the adsorbed hydrogen atoms combine together to form hydrogen molecules instead of generating H+ ions and transferring electrons at the interface. Herein, we report a polarization-induced electric field (PEF) strategy to facilitate FAO on Pd by directing interfacial charge transfer. Pd/TBT-X@SC catalysts with PEF are synthesized with tetragonal phase barium titanate (TBT) as the core, carbonized sucrose as the shell, and palladium nanoparticles as the active sites. The PEF strength is successfully regulated by varying the particle size of TBT. Stronger PEF and proper carbonized sucrose thickness facilitate the interfacial charge transfer on the Pd surface, thereby promoting the electrooxidation of adsorbed hydrogen to H+ ions and converting CO-like species to CO2. Moreover, PEF also induces the formation of electron-deficient Pd, thus reducing the bond strength between Pd and adsorbed intermediate species such as H and CO-like species. Consequently, FAO selectivity, activity, and anti-CO-like poisoning species property of Pd are enhanced by the introduction of PEF. Among all the catalysts, Pd/TBT-100 nm@SC exhibits the highest catalytic activity (7.49 mA·cm–2) and resistance to CO-like poisoning species. This work offers a new strategy for the design of catalysts with high FAO selectivity.
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ACS Catalysis
·
2025
·
IF 13.1
Tao Wang,Qiao Yu,Zhilin Chen,Chao Xiao,Shuming Peng
The active phase for methane combustion is still in debate. Low-temperature CO-FTIR spectroscopy was used to probe the working surface state on a series of Pd/Al2O3 (PdAl) and Pd/silicalite-1 (PdSil) catalysts with different starting states: oxidized, reduced (R), reoxidized (Ro). The surface of prereduced PdAl (Pd0) is transformed to an oxidized state (PdOx) with a CO stretching vibration (νCO) at ∼2157 cm–1 when it is aged in the methane oxidation mixture. The aging-induced transformation from Pd0 to PdOx occurred at 250 °C or above. Although PdSil has multiple kinds of PdOx entities, prereduced PdSil also transformed into PdOx. For PdAl(4)-R-A250, XRD patterns suggest weak bulk oxidation of Pd0 at 250 °C, XPS spectra indicate 28% of surface Pd0 atoms are oxidized, but CO-FTIR spectra confirm all the “top surface” Pd0 atoms are oxidized. It demonstrates the advantage of CO-FTIR spectroscopy in probing the top surface state. Finally, a direct correlation between operando FTIR spectroscopy and low-temperature CO-FTIR spectroscopy was established. Operando FTIR spectra over PdSil during methane oxidation at 250 °C gives two bands at 2124 cm–1 (CO–Pd+) and 2161 cm–1 (CO–Pd2+). After cooling in nitrogen, CO-FTIR spectra give two similar bands at 2134 cm–1 and 2157 cm–1. The “working surface state” can be preserved in CO-FTIR. For PdAl(4), operando FTIR spectra at 250 and 300 °C give no bands of adsorbed CO. Adding CO into the methane oxidation mixture resulted in a single CO–Pd2+ band at 2163 cm–1, which is in accord with their CO-FTIR spectra. For operando FTIR spectroscopy, the observation of the bands of adsorbed CO depends on the accumulation of the CO intermediates, but their accumulation is limited to reaction temperatures below 300 °C and to PdSil (not PdAl). These limitations make low-temperature CO-FTIR spectroscopy more general and sensitive.
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International Journal of Nanomedicine
·
2018
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IF 4.37
Shijie Xu,Fangbo Cui,Dafu Huang,Dinghu Zhang,Anqing Zhu,Xia Sun,Yiming Cao,Sheng Ding,Yao Wang,Eryun Gao,Fenglin Zhang
Background Docetaxel (DOC) is widely used as a chemotherapy drug for various tumors, including gastric cancer (GC), but the clinical application of DOC has been limited due to the hydrophobicity of the drug. We aimed to formulate a multifunctional nanoparticle (NP) system to reduce the side effects of the chemotherapy agent, to promote synergistic therapeutic effects, and to achieve targeted delivery of the therapy. Methods The polyethylene glycol-poly(ε-caprolactone) NPs (PEG-PCL NPs) were prepared by a ring opening copolymerization technique and were then conjugated with a programmed death-ligand 1 (PD-L1) monoclonal antibody (mAb). The effects of the surface coating on particle size, size distribution, zeta potential, drug encapsulation efficiency, loading capacity, and the drug release kinetics were investigated. By using a panel of PD-L1-expressing human GC cell lines and PD-L1-overexpressing cells, we studied cellular uptake, cytotoxic effects, and cellular apoptosis in the presence of PD-L1 mAb-conjugated NPs. Results The characterization of the structure and biological functions of DOC-PEG-PCL-mAb NPs was investigated in vitro. X-ray photoelectron spectroscopy validated the presence of the PD-L1 mAbs on the NP surface. The cellular uptake analysis showed that the antibody-conjugated NPs achieved significantly higher cellular uptake. The results of an in vitro cytotoxicity experiment on three GC lines further proved the targeting effects of the antibody conjugation. In addition, we found that the DOC-PEG-PCL-mAb NPs induced cell apoptosis and enhanced G2-M arrest in cancer cells, indicating the inhibition of microtubule synthesis. When compared with the control groups, DOC-PEG-PCL-mAb NPs are more effective in inhibiting PD-L1 expression in GC cells. Conclusion Our results reported here highlight the biological and clinical potential of DOC-PEG-PCL-mAb NPs using PD-L1 mAbs in GC treatment.
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PubMed
高影响因子
Cancer Cell International
·
2022
·Vol. 22
·期 1
·1-18
·
IF 6.429
Wang Shunxi,Chen Long,Liu Wanqian
Background Ferroptosis have been implicated in tumorigenesis, tumor progression, and chemo- and immuno-therapy in cirrhotic hepatocellular carcinoma (HCC), indicating its association with matrix stiffness and clinical benefit of targeting drugs or immune checkpoint inhibitor. Here, we postulated that increased matrix stiffness reduces ferroptosis and impairs tumor immunity by regulating the expression of ferroptosis- and immune-related genes in HCC, which might be a robust predictor of therapeutic efficacy. Methods Using publicly available tissue microarray datasets, liver cancer rat model, and clinical specimen, ferroptosis-related differential genes in HCV-infected cirrhotic HCC and its mechanical heterogeneous pattern of expression were screened and identified. Further investigation on the underlying mechanism of matrix stiffness-regulated ferroptosis and the expression of immune mediator were performed. Finally, threshold analysis of HCC cases with sorafenib treatment revealed the value of clinical applications of these potential predictors. Results STEAP3 was identified as the ferroptosis-related differential genes in HCV-infected cirrhotic HCC. Stiffer matrix decreased STEAP3 in the invasive front area of HCC and the liver cirrhotic tissue. Contrarily, softer matrix induced STEAP3 in the central area of HCC and the normal liver tissue. Immunological correlation of STEAP3 in cirrhotic HCC showed that STEAP3-mediated immune infiltration of CD4+ T and CD8+ T cells, macrophages, neutrophils, and dendritic cells and HCC prognosis, predicting to regulate immune infiltration. Overexpression of STEAP3 induced ferroptosis and inhibited the expression of immune mediator of PD-L2 on a stiff matrix. Especially, the ferroptosis- and immune-related gene predictive biomarker (FIGPB), including STEAP3 and PD-L2, predicts better clinical benefit of sorafenib in HCC patients. Conclusions This finding identifies matrix stiffness impairs ferroptosis and anti-tumor immunity by mediating STEAP3 and PD-L2. More importantly, coordinated with PD-L2, matrix stiffness-dependent STEAP3 could be applied as the independent predictors to favorable sorafenib response, and thus targeting it could be a potential diagnosis and treatment strategy for HCC.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Xin Dai,Jinqi Wang,Jialiang Zhou,Ning Tang,Senlong Yu,Gongxun Zhai,Hengxue Xiang,Hao Yu,Meifang Zhu
The frequent outbreaks of infectious diseases underscore the critical need for the development of advanced functional protective clothing materials. Herein, we successfully prepared a PE-Pd nonwoven fabric by activating the surface of polyethylene (PE) fibers and constructing Pd-N bonds to ensure the robust attachment of palladium (Pd) nanoparticles to the fabric surface. The PE-Pd fabric demonstrated excellent antibacterial performance, with a minimal Pd addition of just 0.14 %, resulting in 99.9 % inhibition rate against both Escherichia coli ( E. coli ) and Bacillus subtilis ( B. subtilis ). This low concentration ensures high biosafety while retaining potent antibacterial efficacy. The fabric also exhibited a contact angle of up to 104.9 ± 5.9°, significantly reducing microbial adhesion. Additionally, it effectively inhibited biofilm formation, further enhancing its protective properties. Notably, the fabric retained its original moisture permeability, ensuring comfort while maintaining robust barrier functionality. This work presents a promising strategy for the design of next-generation protective clothing, striking an optimal balance between comfort, enhanced safety, and superior barrier performance.
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INORGANIC CHEMISTRY
·
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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CATALYSIS LETTERS
·
2025
·Vol. 156
·期 1
·27
·
IF 2.4
Tian Hongkun,Hu Yuqi,Li Hao
Diisobutyl ketone (DIBK), a high-value chemical with growing market demand, is currently produced as a by-product in methyl isobutyl ketone (MIBK) synthesis, leading to high costs and limited output. This study investigates the one-step synthesis of DIBK from acetone condensation and hydroconversion using Pd/Beta zeolite catalysts. A series of catalysts were prepared via impregnation and systematically characterized by XRD, BET, NH₃-TPD, Py-IR, and XPS. The effects of zeolite type, SiO₂/Al₂O₃ ratio, Pd loading, and reaction conditions on catalytic performance were thoroughly examined. Results demonstrate that Pd/Beta-25, possessing the highest acid site density, optimal Brønsted-to-Lewis acid ratio, and superior Pd dispersion, achieved the best performance: 98.4% acetone conversion and 64% DIBK selectivity under optimal conditions (210 °C, 3 MPa H₂, 9 h). The synergy between abundant acid sites (facilitating condensation) and well-dispersed Pd nanoparticles (enabling hydrogenation) is crucial for promoting the consecutive reaction pathway to DIBK. This work provides fundamental insights and an efficient catalytic system for direct DIBK production, highlighting the advantage of zeolite-based catalysts over conventional Pd/resin systems. Graphical
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ARCHIV DER PHARMAZIE
·
2025
·Vol. 358
·期 12
·e70155
·
IF 3.6
Xinli Wang,Xia Wang,Xuejing Su,Zexin Wang,Yongxiao Sun,Lijun Xie,Xiaoyan Lin
The development of theranostic probes with tumor-specific targeting and high therapeutic efficacy remains a pivotal challenge in precision oncology. Herein, we have successfully developed a new cyclooxygenase-2 (COX-2)-targeted probe compound 2 derived from Rofecoxib. Compound 2 facilitated tumor visualization by a sixfold fluorescence enhancement upon COX-2 binding, while it exhibited minimal background fluorescence under physiological conditions. Moreover, compound 2 monotherapy achieved 53% tumor regression ( p < 0.01). When combined with a programmed cell death protein 1 (PD-1) inhibitor (RMP1-14), concurrent blockade of the COX-2/prostaglandin E2 (PGE2) and PD-1/programmed death-ligand 1 (PD-L1) axes achieved 95% tumor regression ( p < 0.001). Compound 2 involves activating fluorescence by targeting tumor markers COX-2 as well as enhancing therapeutic efficacy. We believe this approach could provide insights for advancing cancer diagnosis and treatment technologies.
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FUEL
·
2025
·
IF 7.5
Zhenzhen Wang,Shufeng Lin,Liujun Wang,Zhe Wang,Bing Lu,Zhonghua Sun,Zhihui Zhang,Mingyang He,Junfeng Qian
The hydrogenation of CO 2 to formic acid (FA) represents a sustainable route for carbon utilization and chemical production, yet it faces challenges in catalytic efficiency, selectivity, and process scalability. Herein, we report a highly efficient catalytic system based on Pd supported on amine-functionalized Zr-SBA-15 (Pd/Zr-SBA-15-AP) for continuous FA synthesis in a fixed-bed reactor. The flake-shaped Zr-SBA-15 support with short mesoporous channels facilitates superior mass transfer. Meanwhile, amine functionalization was identified to serve a dual function: significantly enhancing CO 2 adsorption capacity and modulating the electronic state of Pd to form electron-enriched sites conducive to H 2 activation. The optimized catalyst, 0.3Pd/Zr-SBA-15-AP 3.0 , achieved an exceptional turnover number (TON) of 160 and a turnover frequency (TOF) of 80 h −1 , outperforming the state-of-the-art catalyst under similar continuous-flow conditions. Furthermore, the catalyst demonstrated stable performance over 32 h of continuous operation, underscoring its practical potential. This work provides a scalable strategy for sustainable FA production, effectively bridging laboratory-scale research and industrial application.
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