ACS Catalysis
·
2025
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IF 13.1
Tingting Xiao,Jingrong Li,Jian Li,Qihang Gong,Peikai Luo,Xinluona Su,Haiyang Cheng,Chao Zhang,Fengyu Zhao
The hydrogenolysis of cellulose-derived 5-hydroxymethylfurfural is essential for the production of fuels and chemicals from biomass. Herein, we fabricated a phosphorus-doped Pd/P-TiO2 catalyst for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran. A large number of defects and electron-deficient Ti4+ sites (dTi4+) were formed by doping phosphorus into the TiO2 support, which could promote hydrogen spillover and reactant adsorption. Moreover, the spilled active hydrogen induced the formation of P–O(H)-dTi4+, which acted as a “Brønsted acidic site” to promote the activation of C–O bonds. Consequently, the Pd/P-TiO2 catalyst exhibited superb activity for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran at mild conditions of 150 °C under 1 MPa H2.
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高影响因子
INORGANIC CHEMISTRY
·
2025
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IF 4.7
Qiang-Qiang Ma,Peng Zhou,Yizhen Liu,Zuowei Xie
Transition metal catalyzed selective cage B–H functionalization of carboranes has made significant progress in recent years, giving rise to the efficient synthesis of a large variety of cage B-functionalized carboranes including alkenylation, arylation, alkynylation, borylation, hydroxylation, acyloxylation, amination, and halogenation. However, the mechanisms of these catalytic B–X coupling reactions are not well understood. Herein, we describe the isolation and characterization of the catalytically relevant o-carborane based palladium(II) metallacycle, disclosing the details of Pd-catalyzed B–H functionalization of o-carboranes. As a result, highly selective catalytic B(3,6)-dihalogenation, -dimethylation, and -diarylation of o-carboranes have been achieved.
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PubMed
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2025
·Vol. 23
·期 1
·1-22
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IF 12.6
Liu Yanhong,Gong Liming,Feng Jing,Xiao Congcong,Liu Chenfei,Chen Bohan,Chen Liqing,Jin Mingji,Guan Youyan,Gao Zhonggao,Huang Wei
Immune checkpoint inhibition (ICI) has become the mainstay of immunotherapy for the treatment of renal cell carcinoma (RCC). However, only a small portion of patients exhibit a positive response to PD-1/PD-L1 blockade therapy and the key reason is that RCC belongs to a vascular-rich tumor for promoting immunosuppression. Specifically, the dysfunctional tumor vasculature hinders effector T cell infiltration and induces immunosuppressive tumor microenvironment via the release of cytokine, which attenuates the therapeutic efficacy of ICI. Therefore, regulating abnormal tumor vasculature may be a promising strategy to overcome the immunosuppressive microenvironment and enhance ICI therapy. Here, we propose an NGR peptide-modified actively targeted liposome (Axi/siRNA PD−L1 @NGR-Lipo) to encapsulate the anti-angiogenic agents Axitinib and PD-L1 siRNA to promote tumor vasculature normalization and relieve immune evasion for enhanced anti-tumor immunotherapy. With NGR-mediated tumor homing and active targeting, Axi/siRNA PD−L1 @NGR-Lipo could act on tumor vascular endothelial cells to inhibit neo-angiogenesis, increase pericyte coverage and vascular perfusion, and normalize the structure and function of tumor blood vessels. Meanwhile, it also enhanced immune effector T cells and NK cells infiltration and reduced the proportion of immunosuppressive T cells including MDSC cells and Tregs, thus improving the tumor immunosuppressive microenvironment. Moreover, Axi/siRNA PD−L1 @NGR-Lipo reduced the expression of PD-L1 protein in tumor cells, restored the recognition and killing ability of cytotoxic T cells, and relieved immune evasion. As expected, Axi/siRNA PD−L1 @NGR-Lipo displayed superior anti-tumor and anti-metastatic efficacy in mice bearing RCC. Overall, this study demonstrated the important potential of regulating abnormal tumor vasculature to reshape the immunosuppressive microenvironment and boost ICI therapy, which represents a promising avenue for the synergistic anti-tumor with cancer immunotherapy. Graphical
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
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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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高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Wenyi Wang,Long Tang,Cheng Chen,Xueqin Wang,Yuanyuan Wang,Wencong Sun
Efficient and stable electrocatalysts with low platinum content are crucial for the practical application of fuel cells. The development of Pt-based single atom catalysts (SACs) has emerged as a promising research direction. In this study, we design and prepare a SACs based on MoS 2 with Pt–S–Mo and Pd–S–Mo active sites (Pd, Pt–MoS 2 ) by successively occupying vacancies, while maintaining the individual characteristics of the active sites. The resulting Pd, Pt–MoS 2 catalyst exhibits excellent electrocatalytic activity for oxygen reduction reaction (ORR), long-term stability, and resistance to common poisons (SCN − , S 2− , and methanol) under neutral conditions. Meanwhile, the microbial fuel cell (MFC) equipped with Pd, Pt–MoS 2 exhibits excellent performance in terms of actual electricity generation performance and sewage purification capacity with an ultrahigh power density, average chemical oxygen demand (COD) removal rate, and coulombic efficiency (CE) of 1398.6 ± 43.5 mW m −2 , 96.2 ± 2.2 %, and 22.5 ± 0.5 %, respectively. This strategy will provide new insights into the development of advanced bimetallic as well as polymetallic doped vacancies of MoS 2 SACs.
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高影响因子
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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SENSORS AND ACTUATORS B-CHEMICAL
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2017
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IF 5.401
Lite Yang,Bingjie Xu,Huili Ye,Faqiong Zhao,Baizhao Zeng
A novel molecularly imprinted electrochemical sensor for quercetin (QR) was fabricated via electropolymerization of para -aminobenzoic acid (p-ABA) on a three-dimensional (3D) Pd nanoparticles-porous graphene-carbon nanotubes composite (Pd/pGN-CNTs) modified glassy carbon electrode. The 3D Pd/pGN-CNTs composite was prepared by a facile one-pot hydrothermal method and it exhibited high conductivity, large surface as well as excellent electrocatalysis. The imprinting factor (IF) of MIP sensor toward QR was 3.14, which is higher than those of its analogues (i. e. morin, catechin, rutin, luteolin, and kaempferide). Based on the synergistic effect of the nanocomposite and the molecularly imprinted poly(p-ABA), the resulting electrochemical sensor presented high sensitivity and selectivity. Its linear response range was 0.01–0.50 μM, and the low detection limit was 5.0 nM (S/N = 3). The sensor also showed good reproducibility and stability. It was successfully applied to the detection of QR in food and medicine samples. In addition, theoretical calculations based on density functional theory (DFT) was conducted, and the result indicated that there was strong hydrogen bond between the QR and p-ABA.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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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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高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Qiqi Liang,Yan Fu,Shuaishuai Qiu,Jie Chang
The production of fuel and chemicals from renewable lignin supplies a sustainable chemical engineering process. In this study, Co–Pd bimetallic supported on porous polymer-derived nitrogen-doped carbon spheres (NDCS) was employed for the selective hydrogenolysis of organosolv lignin. Most of the products are phenolic monomers. At optimal conditions, 2.5 MPa H2, 280 °C for 5 h, 86.74% liquefaction of lignin and 36.38 wt % yield of phenolic monomers were obtained. Among these monomer products, 60.83% were identified as 4-hydroxy-3,5-dimethoxyphenylacetic acid (22.13 wt % yield), which is an important pharmaceutical intermediate. With the help of the characterization of catalysts and hydrogenolysis products, the reaction mechanism was proposed. The NDCS provided the prerequisites for metal anchoring and dispersion, and smaller metal particle sizes (2.56 nm) were obtained compared to those of undoped nitrogen carriers. Meanwhile, the synergistic interaction between Pd0 and Co0 promoted the conversion of active hydrogen. With active hydrogen, the C–C and C–O bonds in the lignin were cleaved, and then the active O was transferred to the Pd2+ and Co2+ sites and catalyzed the oxidation of 4-allyl-2,6-dimethoxyphenol to 4-hydroxy-3,5-dimethoxyphenylacetic acid. Lastly, cycling experiments demonstrated the remarkable stability of the catalyst.
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高影响因子
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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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yang Xiao,Chao Qu,Jingjing Zhang,Xi Chen,Wenjin Wang,Xuelong Zheng,Qing Ye
The dissociation of water is essential to water gas shift (WGS) reaction, and the presence of oxygen vacancies can facilitate this key step. Herein, a series of perovskite supported Pd single atoms catalysts were prepared via deposition precipitation method. The incorporation of Pd single atoms can effectively promote the formation of oxygen vacancy on the surface of the catalyst, improving the low temperature reducibility, the ratio of Mn 4 + /Mn 3+ and O ads /O lat compared with support. Among all samples, 0.82 Pd/La 0.5 Ca 0.5 MnO 3 /SBA-15 with the most oxygen vacancies presented 83.6 % CO conversion at 400 °C, specific reaction rate (0.54 mol CO g Pd −1 h −1 ), and TOF (3.77✕10 −2 s −1 ). DFT calculation proved that Pd doping can effectively decreased energy barrier of H 2 O dissociation, and promoted the formation of oxygen vacancies. This work provides experimental and theoretical insights into the rational design of highly active perovskite supported Pd single atom catalysts for WGS reaction.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Jun Wu,Liqian Liu,Xinyue Yan,Gang Pan,Jiahao Bai,Chengbing Wang,Fuwei Li,Yong Li
Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation (HDO) of biomass-derived oxygenates to value-added biofuels is highly desired. An innovative surface microenvironment modulation strategy was used to construct the nitrogen-doped hollow carbon sphere encapsulated with Pd (Pd@NHCS- X , X : 600–800) nanoreactors for catalytic HDO of biomass-derived vanillin in water. The specific surface microenvironments of Pd@NHCS catalysts including the electronic property of active Pd centers and the surface wettability and porous structure of NHCS supports could be well-controlled by the calcination temperature of catalysts. Intrinsic kinetic evaluations demonstrated that the Pd@NHCS-600 catalyst presented a high turnover frequency of 337.77 h –1 and a low apparent activation energy of 18.63 kJ/mol. The excellent catalytic HDO performance was attributed to the unique surface microenvironment of Pd@NHCS catalyst based on structure-performance relationship analysis and DFT calculations. It revealed that pyridinic N species dominated the electronic property regulation of Pd sites through electronic metal-support interaction (EMSI) and produced numerous electron-rich active Pd centers, which not only intensified the dissociation and activation of H 2 molecules, but also substantially improved the activation capability of vanillin via the enhanced adsorption of –C=O group. The fine hydrophilicity and abundant porous structure promoted the uniform dispersion of catalyst and ensured the effective access of reactants to catalytic active centers in water. Additionally, the Pd@NHCS-600 catalyst exhibited excellent catalytic stability and broad substrate applicability for the selective aqueous phase HDO of various biomass-derived carbonyl compounds. The proposed surface microenvironment modulation strategy will provide a new consideration for the rational design of high- performance nitrogen-doped carbon-supported metal catalysts for catalytic biomass transformation.
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