Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Junjing Li,Han Yu,Yongjiao Ding,Liang Wang
In order to improve the metal utilization of the noble metal Pd and the catalytic activity of the reaction, a novel and efficient Pd/Ti 4 O 7 /Ti electrode was prepared by introducing a Ti 4 O 7 intermediate layer for electrocatalytic hydrodechlorination (EHDC) of chlorinated pharmaceuticals and personal care products (PPCPs). The presence of oxygen vacancies (Ov) on the Ti 4 O 7 surface was confirmed by electron paramagnetic resonance (EPR). The results showed that the introduction of Ti 4 O 7 increased the electrochemical active surface area electrode (ECSA) of the Pd/Ti 4 O 7 /Ti electrode, accelerated the electron transfer rate on the catalyst surface, and promoted the generation of electron-rich Pd, which in turn improved the dechlorination efficiency. The Pd/Ti 4 O 7 /Ti electrode had a removal efficiency of 99.6% for florfenicol (FLO) within 180 min. Meanwhile, the removal efficiency of the Pd/Ti 4 O 7 /Ti electrode was still above 95% in seven cycles, which significantly improved the catalytic activity and stability compared with that of the Pd/Ti electrode. In addition, the reaction pathway for the electrocatalytic hydrodechlorination process of FLO at Pd/Ti 4 O 7 /Ti electrode was proposed. The ecotoxicity of the pollutants was also evaluated by the Toxicity Estimation Software Tool (T.E.S.T) model. In this study, an efficient electrocatalyst for EHDC was explored, and the Pd/Ti 4 O 7 /Ti electrode provided strong support for pollutant removal.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Xiaoyu Shi,Yang Yang,Xin Ye,Heng Zhong,Chunling Wang,Fangming Jin
Catalytic conversion of cellulosic biomass into polyols is an effective approach for biomass upgrading. However, the conversion involves cascade reactions which require various catalytic sites cooperation for activating specific steps, resulting in low efficiency. Here, we propose a bifunctional catalyst containing acid sites and hydrogenation capacity for polyol production with cellobiose as the model compound of cellulose. Phosphonic acids (PAs) containing either methyl (MPA) or aminomethyl (NH2MPA) tails were used to tune the Pd/Al2O3 catalyst to form monolayers, thereby modulating the surface physiochemical properties and introducing multiple catalytic sites. An increasing ratio of PdO/Pd and a strong metal–support interaction were observed after PA modification, which could boost the hydrogenation activity for cellobiose. Furthermore, Pd/Al2O3-MPA exhibited excellent hydrolytic hydrogenation activity due to the increase of Lewis acid sites with good durability under hydrothermal conditions by MPA modification, achieving a 78.5% yield of sorbitol at 180 °C for 5 h. A plausible mechanism for enhancing the synergistic effect of Pd and support over Pd/Al2O3-MPA was also proposed. This investigation provides a novel strategy for rationally designing hydrothermally stable bifunctional catalysts to utilize biomass in a more effective way.
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Processes
·
2025
·Vol. 13
·期 3
·853
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IF 2.8
Chenghao Liang,He Liu,Jiahao Liang,Xiaodong Du,Xueqin Tao,Guining Lu
Polybrominated diphenyl ethers (PBDEs), a type of brominated flame retardant, are of global concern due to their environmental persistence, bioaccumulation, toxicity, and resistance to conventional remediation methods. In this study, the electrochemical reduction of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) with Pd/Metal foam electrodes (Ni, Cu, and Ag) was investigated. The effect of Pd loadings was explored, and the results show that Pd loading enhances the debromination performance, with 15.16%Pd/Ni foam exhibiting the best efficiency, followed by 9.37%Pd/Cu and 10.26%Pd/Ag. The degradation mechanisms for Pd/Ni and Pd/Ag are primarily hydrogen atom transfer, while for Pd/Cu, electron transfer dominates. Among the reduction products, Pd/Ni foam shows the highest debromination capability. The impact of electrolytes, current intensity, and bromination degrees of PBDEs was evaluated for 15.16%Pd/Ni. The results reveal that the presence of electrolytes inhibits BDE-47 degradation; the degradation rate of BDE-47 increases with current density, peaks at 4 mA, and decreases as current rises; and 15.16%Pd/Ni foam can effectively degrade PBDEs with varying bromination levels. Additionally, cycling tests show a decrease in efficiency from 94.3% (first cycle) to 56.58% (fourth cycle), attributed to Pd loss and structural damage. The findings offer valuable insights for developing efficient, sustainable catalytic materials for the electrochemical degradation of PBDEs and other persistent organic pollutants.
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JOURNAL OF CATALYSIS
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2024
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IF 6.5
Lei Wang,Badusha Mohamad Ali,Siyang Yu,Sheng Liang,Qingqing Huang,Hao Zhang,Lingyu Zhu,Jianli Wang
Pickering interfacial catalysts incorporated with amphiphilic architecture significantly expand the sustainability of green catalysis systems. In this work, we present precise and well-designed dumbbell-shaped Janus-structured polymeric nanoparticles with one-side anchored palladium clusters (DB-JPP-Pd) as Pickering interfacial catalyst for static hydrogenations. The large wettability difference of each lobe renders the prominent amphiphilicity of the dumbbell-shaped DB-JPP-Pd. The amphiphilic Janus catalyst displays excellent interfacial activity and extensively reduces the interfacial tension from 34.06 ± 0.13 to 20.54 ± 0.31 mN/m, promoting the formation of a more stable Pickering emulsion than that of the bulk PS-Pd catalyst, which can continuously provide a large interfacial area and shorten the molecular mass transfer distance during the reaction process. As a result, the DB-JPP-Pd catalyzed nitroarene reduction reaction exhibits a normalized reaction rate constant (k nor ) of 3.39 min −1 ⋅g −1 ⋅L under static conditions, which is 56.5 times higher than that of bulk PS-Pd. The constructed Pickering interfacial catalysis (PIC) system converts all the nitrobenzene into aniline within three minutes and possesses excellent selectivity in hydrogenations of different nitro aromatics. In addition, the emulsion catalytic system was conveniently recycled for ten consecutive runs. Hence, this unique amphiphilic dumbbell-shaped catalyst effectively develops an efficient static biphasic catalysis system.
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Frontiers in Chemistry
·
2024
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IF 3.8
Zhenghua Zhang,Yang Tian,Wenjun Gao,Yubin Hu,Liangping Luo,Lichang Lei,Shasha Shen,Dan Han
Objectives: Immune checkpoint inhibitors (ICIs) have demonstrated potential in inhibiting the growth of malignant pleural mesothelioma (MPM), and their efficacy is associated with the expression of programmed death-ligand 1(PD-L1). This study evaluated a PD-L1-targeted nanoprobe for detecting PD-L1 expression in a nude mouse model of malignant pleural mesothelioma (MPM).Methods: A PD-L1-binding peptide (WL-12) was conjugated with superparamagnetic iron oxide nanoparticles (SPIONs) to create the nanoprobe WL-12@Fe₃O₄. The nanoprobe’s stability, biotoxicity, targeting ability, and in vivo magnetic resonance (MR) imaging effects were assessed and compared to non-targeted Fe₃O₄ nanoparticles. ΔT2 values and PD-L1 expression were measured in H226 and MSTO-211H tumor tissues over 4 weeks to analyze correlations.Results: The WL-12@Fe₃O₄ nanoprobe demonstrated uniform distribution and a spherical shape, with a larger size (43.82 nm) and lower surface potential (−9.34 ± 0.54 mV) compared to Fe₃O₄ (32.67 nm, −20.20 ± 0.88 mV, P < 0.05). The XPS and FT-IR analysis results indicate the successful coupling of WL-12 with Fe3O4. It was well dispersed in serum and saline and showed no cytotoxicity or organ damage in vivo. The probe selectively accumulated in PD-L1-expressing MPM cells, especially MSTO-211H, and exhibited significantly higher uptake in high PD-L1-expressing H460 cells (930.22 ± 11.75 ng/mL) compared to low PD-L1-expressing A549 cells (254.89 ± 17.33 ng/mL, P < 0.05). Tumor iron levels in the WL-12@Fe₃O₄ group were significantly elevated (141.02 ± 17.33 μg/g) compared to controls (36.43 ± 3.56 μg/g, P < 0.05), with no significant differences in other organs (P > 0.05). The T2 values of H226 and MSTO-211H tumors decreased after probe injection, with ΔT2 values significantly higher in the targeted group than the nontargeted group (P < 0.05). ΔT2 values increased over 4 weeks, correlating strongly with PD-L1 expression (P < 0.05).Conclusion: The PD-L1-targeted nanoprobe with MRI is a promising tool for noninvasive, real-time assessment of PD-L1 expression in MPM.
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MICROCHEMICAL JOURNAL
·
2024
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IF 4.9
Ziping Li,Qijie Mo,Guiyan Li,Xian Wang,Junjie Shao,Yao Zhang,Jian Chen,Zhijun Chen,Jingwen Tan,Zhenji Wang,Yijin Shu,Qingsheng Gao
Supported metal nanomaterials have great potential in catalytic sensing, but the poor selectivity and easy aggregation of noble metals limit their development in non-enzyme sensing applications. Herein, this research focuses on the metal-support interactions of Pd supported on PCN-222, exploring the role of abundant porphyrin groups on the PCN-222 surface and the tuning of Pd composition to enhance electron configuration. Through the anchoring of PCN-222 surface to Pd species and utilizing the confining effect of open channels, the Pd@PCN-222 nanostructures with uniform particle size of Pd were successfully obtained. Strong electron interaction can enhance the catalytic activity of Pd@PCN-222 towards reaction, while increasing the Pd loading can improves the sensitivity of the sensors in the high concentration of H 2 O 2 . Combining the above two points, 0.29 %-Pd@PCN-222 exhibits a low detection limit of 0.27 μM and a wide linear range of 1–1000 μM in H 2 O 2 sensing via using a colorimetric method. Experimental and theoretical results show that Pd@PCN-222 exhibit strong p - d orbital coupling and adsorption, and rapid catalytic kinetics towards H 2 O 2 , enhancing the overall catalytic process. At the same time, DFT calculations are used to simulate the material surface and sensing process, which also enrich the research content of MOF materials in sensing. From the structure-performance relationships to the directly analyze the H 2 O 2 in real samples, this work is expected to provide some guidance for the development of efficient sensing systems.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Yuhao Yang,Chunhua Wang,Jiani Cai,Ying-Ya Liu,Zhiquan Yu,Zhichao Sun,Yao Wang,Anjie Wang,Chong Peng
Selective hydrogenation of phenol to cyclohexanone is of great significance for the production of value-added chemical intermediates and products. Pd/MIL-100(Cr), featuring highly dispersed Pd nanoparticles (∼2.5 nm), were synthesized using a double-solvent impregnation method followed by NaBH4 reduction. During aqueous-phase phenol hydrogenation, the catalyst achieved full conversion with 98.3% selectivity toward cyclohexanone within 1 h at 0.1 MPa and 100 °C. The catalyst exhibited high stability, maintaining performance up to 5 cycles without deactivation. The Lewis acidity of MIL-100(Cr) significantly influenced the phenol hydrogenation selectivity. By incorporation of Al, V, and Ce species into the MIL-100(Cr) framework, cyclohexanone selectivity in phenol hydrogenation was found to increase with the amount of Lewis acid sites (LAS). The acid properties of the Pd/MIL-100 catalysts were investigated using NH3-TPD, pyridine-adsorbed FT-IR, and EPR probe molecules. The interaction between Pd nanoparticles and the coordinatively unsaturated sites from the trimeric clusters of MIL-100 was found to be crucial in determining the Lewis acidity of the Pd/MIL-100 catalysts. Demonstrating a synergistic effect between the Pd and LAS, Pd/MIL-100(Cr) emerges as a promising candidate for the selective hydrogenation of phenol to cyclohexanone.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
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IF 8
Yijun Chen,Meina Cheng,Long Jin,Hailiang Yang,Sanjian Ma,Zixia Lin,Guoliang Dai,Xin Liu
The Fenton reaction is recognized as an effective technique for degrading persistent organic pollutants , such as the emerging pollutant trimethoprim (TMP). Recently, due to the excellent reducibility of active hydrogen ([H]), Pd–H 2 has been preferred for Fenton-like reactions and the specific H 2 activation of Pd-based catalysts. Herein, a heterogeneous Fenton catalyst named the hydrogen-accelerated oxygen reduction Fenton (MHORF@UiO-66(Zr)) system was prepared through the strategy of building ships in the bottle. The [H] has been used for the acceleration of the reduction of Fe(III) and self-generate H 2 O 2 . The systematic characterization demonstrated that the nano Pd 0 particle was highly dispersed into the UiO-66(Zr). The results found that 20 mg L −1 of TMP was thoroughly degraded within 90 min in the MHORF@UiO-66(Zr) system under conditions of initial pH 3, 30 mL min −1 H 2 , 2 g L −1 Pd@UiO-66(Zr) and 25 μM Fe 2+ . The hydroxyl radical as well as the singlet oxygen were evidenced to be the main reactive oxygen species by scavenging experiments and electron spin resonance . In addition, both reducing Fe(III) and self-generating H 2 O 2 could be achieved due to the strong metal-support interaction (SMSI) between the nano Pd 0 particles and UiO-66(Zr) confirmed by the correlation results of XPS and calculation of density functional theory. Finally, the working mechanism of the MHORF@UiO-66(Zr) system and the possible degradation pathway of the TMP have been proposed. The novel system exhibited excellent reusability and stability after six cyclic reaction processes.
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CERAMICS INTERNATIONAL
·
2025
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IF 5.6
Bangqia Huang,Qingge Feng,Zequan Li,Qihua Liang,Guo-Dong Li
Given the potential hazards posed by triethylamine (TEA) to human health and environmental safety, it is crucial to have real-time and efficient detection methods in place. However, the low reactivity of TEA poses a challenge in achieving effective detection at low temperature. Hence, a high-performance sensor for detecting TEA was developed using Pd-doped WO 3 prepared through a one-step electrospinning method. The sensor based on 1.0 wt% Pd-WO 3 exhibited exceptional performance in detecting TEA at low temperature (100 °C), showing a response of 246 to 20 ppm. Additionally, it demonstrated a low detection limit (0.03 ppm) and excellent selectivity characteristics. The outstanding sensing capability can be ascribed to the noble metal electron sensitization and spillover effects, which enhance the interaction between chemisorbed oxygen and TEA gas by adjusting the Fermi level of 1.0 wt% Pd-WO 3 . This adjustment achieves surface electron redistribution and optimizes interfacial atomic transport, while also reducing the activation energy required for gas sensing, thereby lowering the operating temperature.
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Journal of Water Process Engineering
·
2024
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IF 6.3
Yijun Chen,Hailiang Yang,Sanjian Ma,Meina Cheng,Zixia Lin,Long Jin,Xin Liu
As a representative antibiotic, trimethoprim (TMP), the emerging pollutant has been frequently detected in water bodies, and its potential harm has aroused the attention of society. Although the emerging pollutant could be efficiently degraded by the advanced oxidation process (AOP) represented by the Fenton reaction , both the problem of iron sludge disposal and the safe use of H 2 O 2 have plagued the further promotion of this technology. The H 2 (precursor of the active hydrogen [H]) and catalyst Pd/UiO-66(Zr) were introduced into the Fenton reaction in this paper. It was found that the process of reducing Fe(III) and self-generating H 2 O 2 could be facilitated due to the reduction of [H]. Under certain reaction conditions (initial pH 3, trace total iron 25 μM, H 2 30 mL·min −1 , catalyst 2 g·L −1 ) and without H 2 O 2 , a Fenton-like system was constructed, named MHORF-UiO-66(Zr). While achieving zero iron sludge discharge, 100 % of 20 mg·L −1 TMP was rapidly degraded within 1 h. It was found that the degradation of TMP could be attributed to the attack of singlet oxygen and hydroxyl radical . Furthermore, the performance changes of catalyst before and after six rounds of reactions were studied and it was found that Pd/UiO-66(Zr) had excellent and stable catalytic performance.
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Science Advances
·
2024
·Vol. 10
·期 10
·
IF 11.7
Rui Feng,Yong-Qi Zhen,Dongbo Wu,Lian Sun,Jin-Bu Xu,Xiaohuan Li,Lan Zhang,Feng Gao
Achieving regioselective synthesis in complex molecules with multiple reactive sites remains a tremendous challenge in synthetic chemistry. Regiodivergent palladium-catalyzed C─H arylation of complex antitumor drug osimertinib with various aryl bromides via the late-stage functionalization strategy was demonstrated here. This reaction displayed a switch in regioselectivity under complete base control. Potassium carbonate (K2CO3) promoted the arylation of acrylamide terminal C(sp2)-H, affording 34 derivatives. Conversely, sodium tert-butoxide (t-BuONa) mediated the aryl C(sp2)-H arylation of the indole C2 position, providing 27 derivatives. The derivative 3r containing a 3-fluorophenyl group at the indole C2 position demonstrated similar inhibition of EGFRT790M/L858R and superior antiproliferative activity in H1975 cells compared to osimertinib, as well as similar antiproliferative activity in A549 cells and antitumor efficacy in xenograft mouse model bearing H1975 cells. This approach provides a “one substrate–multi reactions–multiple products” strategy for the structural modification of complex drug molecules, creating more opportunities for the fast screening of pharmaceutical molecules.
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Acta Pharmaceutica Sinica B
·
2024
·
IF 14.7
Chongzheng Yan,Ying Liu,Guozhi Zhao,Huatian Yang,Huaiyou Lv,Genju Li,Yuhan Li,Yaqing Fu,Fengqin Sun,Yafei Feng,Yizhe Li,Zhongxi Zhao
Cuproptosis shows enormous application prospects in lung metastasis treatment. However, the glycolysis, Cu + efflux mechanisms, and insufficient lung drug accumulation severely restrict cuproptosis efficacy. Herein, an inhalable poly(2-( N -oxide- N , N -diethylamino)ethyl methacrylate) (OPDEA)-coated copper-based metal–organic framework encapsulating pyruvate dehydrogenase kinase 1 siRNA (siPDK) is constructed for mediating cuproptosis and subsequently promoting lung metastasis immunotherapy, namely OMP. After inhalation, OMP shows highly efficient lung accumulation and long-term retention, ascribing to the OPDEA-mediated pulmonary mucosa penetration. Within tumor cells, OMP is degraded to release Cu 2+ under acidic condition, which will be reduced to toxic Cu + to induce cuproptosis under glutathione (GSH) regulation. Meanwhile, siPDK released from OMP inhibits intracellular glycolysis and adenosine-5ʹ-triphosphate (ATP) production, then blocking the Cu + efflux protein ATP7B, thereby rendering tumor cells more sensitive to OMP-mediated cuproptosis. Moreover, OMP-mediated cuproptosis triggers immunogenic cell death (ICD) to promote dendritic cells (DCs) maturation and CD8 + T cells infiltration. Notably, OMP-induced cuproptosis up-regulates membrane-associated programmed cell death-ligand 1 (PD-L1) expression and induces soluble PD-L1 secretion, and thus synergizes with anti-PD-L1 antibodies (aPD-L1) to reprogram immunosuppressive tumor microenvironment, finally yielding improved immunotherapy efficacy. Overall, OMP may serve as an efficient inhalable nanoplatform and afford preferable efficacy against lung metastasis through inducing cuproptosis and combining with aPD-L1.
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