CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xinyu Zhang,Hui Liu,Chenyu Wang,Yuan Gao,Shiqi Zhao,Mengyao Mu,Ke Ren,Yufang Gong,Qing Fan,Xiao Sun
Biodegradable Two-dimensional (2D) nanomaterials have attracted tremendous interest in biomedical application. Herein, a biodegradable ferrous sulfide nanosheet with ultrathin structure and uniform size was developed. Following its development, the application of the self-enhanced photothermal nanoplatform (FMPN) in vivo by combining Mn-DOTA and dimeric PD-L1 affibody for targeted dual-mode magnetic resonance imaging (MRI) guided synergistic tumor therapy is explored. Dual-contrast enhanced subtraction imaging (DESI) was used to evaluate the excellent T1-T2 MRI ability of FMPN. FMPN displayed excellent photothermal conversion efficiency (η = 40.33 %) and biodegradability, thus had good tumor photothermal therapy effects with good biosafety. In addition, FMPN with pH-responsive Fe 2+ release can effectively induce tumor cell ferroptosis, further intensifying PTT and subsequent immunologic cell death. PD-L1 affibody could endow this nanoplatform with efficient tumor targeting, terminating T cells’ immune suppression by effectively blocking the interaction between PD-1 and PD-L1. Systemic delivery of FMPN significantly inhibited tumor progression in primary, metastatic and abscopal tumors, and showed obvious dual-mode MRI enhancement. Therefore, this nanoplatform exhibited promising potential for MRI-guided synergistic ferroptosis/photothermal/immunotherapy.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Linsen Li,Zhuwei Yang,Hui Xiong,Ming Ma,Riguang Zhang,Zhao Jiang
The NECZ/12H-NECZ (N-ethylcarbazole/dodecahydro-N-ethylcarbazole) system is one of the commercially promising liquid organic hydrogen carriers (LOHCs). However, the dehydrogenation reaction of 12H-NECZ is still the bottleneck of the whole hydrogen storage and release process, possessing a relatively low hydrogen release rate. In this study, one kind of C3N4 (carbon nitride) mesoporous nanosheet material with abundant N vacancies was fabricated by the thermal treatment of trace S-doped C3N4, and a series of Pd-based catalysts were prepared by the impregnation reduction method. The Pd/S0.03-C3N4-Nv550 (treated by S-doped and N) catalyst with abundant N vacancies showcases the most outstanding catalytic performance, achieving a 5.41 wt % hydrogen release amount as well as 81.09% NECZ selectivity at 90 min. Combined with the experimental and computational results, the presence of trace S does not lead to structural collapse of the material and interestingly induces the generation of high concentrations of N vacancies. The N vacancies greatly facilitate the dispersion of loaded metals, offering more active sites; meanwhile, the existence of N vacancy weakens the electronic localization of C3N4 carriers, modulates the electronic structure of active metal Pd, and promotes the activation of reactants and intermediates. What is more, the Pd/S0.03-C3N4-Nv550 catalyst shows excellent stability during long-term cycle tests. It provides some reference values for the design of LOHC dehydrogenation catalysts.
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ACS Sustainable Chemistry & Engineering
·
2024
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IF 7.1
Jun Wu,Liqian Liu,Xinyue Yan,Tingting Wang,Gang Pan,Jiahao Bai,Yong Li
Catalytic hydrodeoxygenation (HDO) of bio-oil is an effective and challenging route to the efficient utilization of biomass with rich oxygen-containing groups. Herein, highly dispersed Pd nanoparticles (NPs) anchored on a N-doped hollow carbon sphere (NHCS) were constructed to effectively catalyze the chemoselective HDO of bio-oil-derived vanillin. The optimized Pd/NHCS-900 catalyst presented a high 99% conversion and 98% selectivity to 2-methoxy-4-methylphenol (MMP) within 45 min under very mild conditions of 50 °C and 1 atm H2. The incorporated N species in the NHCS support and its hierarchical porous structure facilitate the dispersion and stabilization of Pd NPs, resulting in the formation of highly dispersed Pd NPs with excellent structure stability. Moreover, the presence of a strong electronic metal–support interaction between N and highly dispersed Pd NPs produced the surface electron-rich active Pd NPs, which could enhance the adsorption and activation of reactants, thereby exhibiting high intrinsic catalytic activity with a large turnover frequency (TOF) of 1700.3 h–1. Kinetic study and density functional theory (DFT) calculations demonstrated the HDO reaction pathway and the corresponding reaction mechanism. These findings pave the way for the development of efficient and stable metal catalysts for sustainable biomass conversion.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 6
·1-11
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IF 5.3
Hao Xuanxuan,Liu Zhimin,Zheng Tongtong,Fan Yunfeng,Hu Leqian
A signal-amplified platform was designed to construct a label-free electrochemical aptasensor for lead ions (Pb 2+ ) assay. First, flower-like molybdenum disulfide-supported AuNPs (AuNPs@MoS 2 ) nanocomposites were synthesized and used as substrates for modifying the electrode. The AuNPs@MoS 2 material possessed large surface area and superior biocompatibility, which was beneficial to improve the loading amount of the complementary DNA (cDNA) and amplified the response signal. Importantly, the prepared core–shell Pt@Pd bimetallic nanoparticles (Pt@PdNPs) were used to conjugate with redox marker thionine (Thi) and aptamer (Apt) for further signal amplification; the obtained signal probes (Thi-Pt@PdNPs-Apt) were connected by the cDNA assembled on the electrode through DNA hybridization. Differential pulse voltammetry was performed to monitor the signal of Thi. After incubating of aptasensor with Pb 2+ , the specific recognition of Pb 2 + and Apt resulted in the dissociation of aptamer-cDNA complex, thereby the Thi-Pt@PdNPs-Apt separated from the electrode surface and decreased current response was obtained. The prepared electrochemical sensor exhibited linear response to Pb 2+ in the range 5.0 × 10 −4 –100 nM and a detection limit of 1.0 × 10 −4 nM was achieved. The sensor was applied to the determination of Pb 2+ in actual sample with high sensitivity and accuracy, demonstrating potential applications in heavy metal monitoring. Graphical Abstract
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Keyan Liu,Wei Feng,Yanru Li,Donglai Han,Tianna Wu,Kaiyue Li,Shuo Yang
Surface-enhanced Raman spectroscopy (SERS) with enormous advantages has emerged as a powerful tool for both highly sensitive structural detection of analytes and various imaging applications. A notable advancement in the realm of multifunctional SERS substrates is the integration of magnetic nanoparticles endowed with magnetic manipulation capabilities and noble metal nanoparticles exhibiting plasmonic resonance properties. This synergistic combination offers substantial practical benefits for trace analysis across diverse fields. In this paper, a new paradigm of Fe 3 O 4 @PEI-DTC-Ag (Fe 3 O 4 @PD-Ag) photomagnetic nanocomposites based on magnetic Fe 3 O 4 nanoparticles (NPs), the noble metal silver quantum dots (Ag QDs) and the adhesive layer polyethyleneimine dithiocarbamate (PEI-DTC) for convenient recycling and ultrasensitive SERS detection was developed by engineering hydrothermal and seed-growth methods. The SERS performance of the Fe 3 O 4 @PD-Ag substrates with varying amounts of Ag was evaluated by detecting 4-aminothiophenol (4-ATP). Among the tested samples, Fe 3 O 4 @PD-Ag-4 with a silver solution volume of 200 ml exhibited the optimal performance, showcasing an enhancement factor ( EF ) of 4.418 × 10 5 . Moreover, the relative standard deviations (RSDs) were calculated to be less than 11.5 %, demonstrating the SERS substrates exhibit good uniformity and spectral reproducibility. Of note, the SERS substrate has demonstrated successful trace detection of thiram molecules, achieving a limit of detection (LOD) of up to 10 -9 M. The intensity of SERS signals shows a linear correlation with the logarithm of thiram concentration, ranging from 10 -4 to 10 -9 M, thus providing compelling evidence for quantitative detection. Importantly, the Fe 3 O 4 @PD-Ag-4 SERS substrate also showcases outstanding performance for detecting thiram in real food, underscoring its significant potential for application in food safety monitoring.
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Sustainable Materials and Technologies
·
2024
·
IF 8.6
Yijun Chen,Meina Cheng,Hailiang Yang,Sanjian Ma,Long Jin,Zixia Lin,Xin Liu
The traditional Fenton process has two issues that hinder its further application and promotion. One is the generation of large amounts of iron sludge. The other is the safe storage and transport of explosive H 2 O 2 . The problems could be solved by accelerating to regenerate Fe(II) and realizing to self-generate H 2 O 2 . The key to the solution lies in the use of reducing active hydrogen [H] to supply electrons. The effect of different loading methods of Pd 0 nanoparticles (NPs), active centres for [H] generation, on the catalytic performance is unknown. Herein, the Pd/UiO-66(Zr) (Pd 0 NPs loaded on the surface of UiO-66(Zr)) and Pd@UiO-66(Zr) (Pd 0 NPs confined into the pores of UiO-66(Zr)) were synthesized. It confirmed that the [H] could be used to promote to regenerate Fe(II) and self-generate H 2 O 2 . Using only a trace amount of ferrous (25 μM) and without H 2 O 2 , the trimethoprim (20 mg·L −1 ) could be thoroughly removed within 90 min. Moreover, the stability of Pd@UiO-66(Zr) was slightly superior to that of Pd/UiO-66(Zr) because of the confinement effect of pore wall on Pd 0 NPs, as well as the interception effect on the intermediate products that can be complexed with Pd 0 NPs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yingna Wang,Zilong Liu,Yuanpei Lan,Chaoyi Chen,Wei Zhang
The removal of small amounts of phenylacetylene from styrene is a crucial step in the production of high-quality styrene feedstocks. In the presence of a large amount of styrene and a small amount of phenylacetylene, achieving and maintaining high selectivity of styrene remains a significant challenge. In this work, a catalyst denoted as Pd 1.25 -Fe-N-C/VC was designed and synthesized with remarkably low Pd loading (the actual Pd content was 0.96 wt%). The catalyst exhibited a satisfactory selectivity for styrene (>95 %) and maintained high selectivity levels (>90 %) in the semi-hydrogenation of phenylacetylene even with prolonged reaction time. Pd nanoparticles (NPs) were well distributed and securely anchored onto the Fe-N-C/VC support with a hierarchical mesoporous structure, which obtained from the pyrolysis of a hexagonal star-like Fe-doped zeolitic imidazolate framework with vitamin C surfactant (Fe-doped ZIF/VC). The remarkable catalytic properties may be partly ascribed to the effective synergy effect of the uniformly well-dispersed Fe-N x (x represents the coordination number) with Pd active centers, which could modulate the adsorption kinetics of the reactant alkynes and alkenes and thus enhancing the selectivity towards styrene. Meanwhile, the hierarchical mesoporous structure is beneficial for the mass transfer, which can effectively promote the interactions between the reactants and active centers. Possible mechanism for the selective hydrogenation of phenylacetylene catalyzed by Pd 1.25 -Fe-N-C/VC was also illustrated. Moreover, the Pd 1.25 -Fe-N-C/VC catalyst exhibited sustained catalytic activity and selectivity even after four continuous cycle tests, showing notable reusability and stability. This work may offer a promising approach for creating highly efficient Pd-based catalysts with remarkably low Pd loading for phenylacetylene semi-hydrogenation.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Feng Xie,Guanghuan Li,Feng Yan,Chengbin Xiao,Pengju Wang,Xuehua Shen,Biao Yang,Han Lin,Huarong Luo,Zuotai Zhang
Solid–liquid biphasic absorbents are a promising solution for overcoming the high-energy consumption challenge faced by liquid amine-based CO2 capture technologies. However, their practical applications are often hindered by difficulties in separating viscous solid-phase products. This study introduces a novel nonaqueous absorbent system (PD/PZ/NMP) composed of 4-amino-1-methylpiperidine (PD), piperazine (PZ), and N-methyl-2-pyrrolidone (NMP), engineered to produce easily separable powdery products. The PD/PZ/NMP absorbent achieves a CO2 loading of 0.86 mol-CO2/mol-amine, with 91% of CO2 concentrated in the solid phase. It demonstrates excellent cyclic stability, maintaining a regeneration efficiency of 91% after five regeneration cycles, and reduces energy consumption by 52% compared with the conventional monoethanolamine absorbent. Remarkably, PZ plays a crucial role in regulating the crystal composition of solid-phase products, transforming them from a viscous state to a crystalline powder. Characterization and density functional theory analysis explain the crystal-phase regulation mechanism: PD absorbs CO2 to form zwitterions (PDH+COO–), affording viscous products, and PZ forms protonated amines (PZH+) and monocarbamates (PZCOO–), which interact with PDH+COO– via hydrogen bonding to form a crystalline powder. These findings demonstrate the CO2 capture efficacy of the PD/PZ/NMP absorbent and provide a robust theoretical framework for fabricating solid–liquid biphasic absorbents tailored for practical applications.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2025
·
IF 5.9
Kan Li,Shengbin Gui,Ningning Wang,Xiao Li,Chunqin Zhao,Mingyu Liu,Zhen Zhang
Intravenously administered nanoparticles (NPs) often bind with plasma proteins, forming protein corona that prompt rapid systemic clearance, a primary challenge in nanomedicine. In this study, we developed a pH- and GSH-sensitive “stealth” nanodelivery system, PTX@NPs-aPD1-IL, for sequential drug release. By using a biocompatible choline-based ionic liquid (IL) as the coating for NPs, the interaction and adsorption of NPs with serum proteins were reduced, achieving targeted delivery to the lung organ and increasing drug accumulation. In the weakly acidic extracellular tumor microenvironment (pH 6.5), the anti-PD-1 antibody (aPD-1) was first released to block the PD-1/PD-L1 pathway and restore the immunocidal function of T cells. In the highly reductive intracellular environment of tumor cells, the disulfide bonds were cleaved, causing NPs to rupture and release paclitaxel (PTX). It induced tumor cell apoptosis and triggered immunogenic cell death (ICD), promoted dendritic cells (DCs) maturation and activated T cells for chemo-immunotherapy. In the mouse orthotopic lung cancer model, PTX@NPs-aPD1-IL exhibited superior efficacy to other treatment groups at the same dose. This was due to the significantly increase in the release of immune factors, including TNF-α and IFN-γ, and the promotion of CD8 + T cells recruitment, which induced a stronger immune response, and thus enhanced the anti-lung cancer effect. In summary, PTX@NPs-aPD1-IL provided a promising strategy for effective chemo-immunotherapy for lung cancer through sequential release profile.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Abubakar Yusuf,Yong Ren,Yun Liu,Li Shi,Zhiyu Xiao,Run Pan,Zheng Wang,Hainam Do,Jianrong Li,Jun He
The efficient treatment of methane emissions from natural gas-powered engines is necessary due to the high potency and global warming potential of methane. Promoters are often employed to enhance catalysts’ performance and stability for methane oxidation. It is therefore important to understand the impact of promoters on Pd activity, especially under practically relevant conditions. Here, we report the enhancement and inhibition effect of promoters (ZrO 2 , CeO 2 , and TiO 2 ) on the sulfur resistance and regeneration of alumina-supported Pd catalysts for complete methane oxidation in the presence and absence of moisture. The type of promoter employed and the presence of moisture influence the type of sulfur species formed on the alumina-supported Pd catalysts, as well as their catalytic performance and regeneration. Whereas ZrO 2 enhances both the activity and SO 2 resistance and enhances the regeneration of the poisoned catalysts under both dry and wet reaction conditions, more stable sulfate species are formed in the presence of CeO 2 and TiO 2 , inhibiting both the catalysts’ performance and regeneration. In addition, the presence of ZrO 2 protects the active Pd sites from progressive deactivation over sulfur poisoning and regeneration cycles. The results of this work provide insights into how promoters influence the activity, sulfur poisoning and regeneration of methane oxidation catalysts in the presence and absence of moisture, which have implications for the practical design of industrially relevant catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuanyan Luo,Tao Zhou,Costas Molochas,Yongkang Tan,Xiaoting Huang,Zhenyu Chen,Jinliang Zhu,Panagiotis Tsiakaras,Peikang Shen
Pt-Pd-Ni polyhedral nanobelt (PNBs) composite catalysts are synthesized in presence of tungsten hexacarbonyl [W(CO) 6 ] by a simple solvothermal method, combining both higher specific surface area and more index active site than the corresponding single-structure catalysts. The thermal decomposition of W(CO) 6 plays a crucial role in the morphology formation. The tenuous composite with a moderate nanobelt width of 7.46 nm formed after heating for 6 h (Pt-Pd-Ni PNBs2) shows better ORR performance and durability than the ternary (Pt-Pd-Ni) and binary (Pt-Pd) single structures. It exhibits a mass activity of 1.49 (A mg Pt −1 ), which only degrades by about 10.63 % after 50,000 durability cycles. The metal regulatory effects induced by the carbonyl compounds cause the contraction of the Pt-Pt bonds. Density functional theory calculations indicate that the compressive strain of Pt-Pd-Ni PNBs2 leads to a decrease in the d-band center and overpotential negatively shifted, thus provide a more sufficient and faster ORR proceeding process in thermodynamics, facilitating a higher energy conversion efficiency.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Jianfeng Wang,Jintian Ren,Zhen Xu,Qiang Wei,Fan Yang
The synergistic effects in bimetallic catalysts drive significant interest for hydrogenation catalysis. In this work, a series of Pd-Ru bimetallic catalysts supported on N-doped porous carbon were synthesized, with the optimized Ru₁Pd₁/NPC-1 exhibiting outstanding pyridine hydrogenation performance. Quantitative conversion was achieved under mild reaction (room temperature, H 2 balloon pressure), accompanied by remarkable substrate adaptability and recyclability. The introduced N species and hierarchical porous structure in the NPC carrier synergistically facilitate the dispersion and stabilization of metal nanoparticles, thereby forming highly dispersed metallic clusters with exceptional structural robustness. Furthermore, the formation of a Pd-Ru bimetallic alloy establishes novel active centers that strengthen reactant adsorption and activation, ultimately leading to superior catalytic activity. Density functional theory (DFT) calculations corroborate that the bimetallic system exhibits optimized adsorption energy and accelerated piperidine desorption efficiency. These results establish a foundation for designing stable and efficient metallic catalysts enabling sustainable pyridine conversion.
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