JOURNAL OF CONTROLLED RELEASE
·
2023
·
IF 10.8
Tiantian Liu,Zehang Zhou,Mengxing Zhang,Puxin Lang,Jing Li,Zhenmi Liu,Zhirong Zhang,Lin Li,Ling Zhang
The cuproptosis cell death pathway brings fresh opportunities for tumor therapy. However, efficient and targeted cuproptosis induction in tumors is still a challenge. Unfortunately, the well-known cuproptosis initiator, disulfiram and copper complex (DSF/Cu 2+ ), also increases PD-L1 level in tumors, which may diminish the final therapeutic outcome. In this study, DSF/Cu 2+ -loading MXene nanosheets are coated with PD-1 overexpressing T cell membrane to generate CuX-P system. CuX-P could recognize and stick to PD-L1 on tumor cells like a patch, which promotes the endocytosis of both CuX-P and PD-L1 by tumor cells. Following internalization and release of DSF/Cu 2+ in the cytoplasm, PD-L1 expression is upregulated. However, due to the presence of CuX-P in the tumor microenvironment , the then supplemented PD-L1 on tumor surface again binds CuX-P for internalization. This feedback loop keeps blocking and consuming the PD-L1 on tumor surface and promotes the enrichment of CuX-P in tumors to induce cuproptosis. After CuX-P treatment with laser irradiation, strong anti-tumor immune responses are stimulated in a mouse model with triple-negative breast cancer. Thus, this study develops a tumor-targeted biomimetic system that offers simultaneous cuproptosis killing, photothermal therapy (PTT) and immunotherapy in mice.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jun Zhang,Chunyuan Wang,Shiyu Lu,Shuyue Liu,Pingjuan Liang,Huan Yi,Mengjie Li,Meng Jin,Rong Wang,Guangming Jiang
Enhancing the enrichment behavior of low-concentration chlorinated organic pollutants remains a significant challenge in electrocatalytic hydrodechlorination (EHDC) technology. Metal-loaded hollow nanoarchitecture has emerged as a promising nanoreactor to improve reaction enrichment behavior because of its tailorable microenvironments and electronic properties. Herein, a structural engineering strategy is developed to synthesize yolk-shell structured TiN spheres supported Pd nanoreactors (Pd/YS-TiN) with confined mesoscopic spaces. Characterization by multiple techniques reveals that the yolk-shell structure of YS-TiN, with high specific surface area (139.0 m 2 /g) and appropriately mesoporosity (6.9 nm), exposes numerous Pd nanoparticles (∼4.0 nm) on outer/inner surface of the shell and yolk-core solid sphere, ensuring an efficient utilization of active sites for enhancing the 2,4-DCP detoxification. Consequently, the structurally optimized Pd/YS-TiN nanoreactor consistently displays maximum reaction kinetics, dechlorination degree, faradaic current density, H* utilization and product selectivity, surpassing hollow TiN-supported Pd and Pd/C catalysts. The super EHDC performance of 91.8 % 2,4-DCP conversion, a specific activity of 1.68 min −1 mol Pd −1 , and a mass activity of 6.06 min −1 g Pd −1 is obtained at −0.85 V and 180 min, outperforming most reported catalysts. Combining experimental and density functional theory results, the exceptional reaction enrichment behavior of Pd/YS-TiN originates from (1) alleviating the overstrong adsorption of product phenol through strong metal-support interactions and (2) enhancing mass transport efficiency facilitated by the local concentration gradient and mesoporous shell. This study elucidates how metal-support interactions and mass transport synergistically enhance reaction enrichment behavior, showcasing potential benefits in environmental remediation applications.
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Catalysis Science & Technology
·
2023
·Vol. 14
·期 2
·334-342
·
IF 5
Zhou Yang,Ru Wang,Hongji Liu,Zhou Chen,Xiaoli Hu,Limin Sun,Weikun Lai,Yunyun Dong,Weiping Fang,Xiaodong Yi
Selective hydrogenation is a significantly important catalytic process in many industrial processes, where Pd-based catalysts are the most commonly used. Herein, the surface properties of γ-Al2O3 were modified by the layered flower-like architectures of alkaline MgO using a simple hydrothermal method. Then, a series of Pd/Al2O3–MgO catalysts were prepared by an incipient wetness impregnation method for the selective hydrogenation of isoprene. The results showed that the Pd/Al2O3–0.12MgO catalyst exhibited superior catalytic performance with a high activity (93%) and high selectivity (99%) for the semi-hydrogenation products. Systematic studies have demonstrated that the support effect plays an important role in dispersing and stabilizing palladium particles. The reasons for the improved catalytic performance were attributed to the high dispersion of Pd nanoparticles, the changed electronic structure of Pd, and the strong interaction between Pd nanoparticles and supports. This work opens a simple route to regulate the electronic properties of active metal sites via support modification for selective hydrogenation reactions.
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Molecular Catalysis
·
2023
·
IF 4.6
Xuewu Ji,Guirong Bao,Peng Gao,Jia Luo,Dequan Chen,Zhen Fang
Vanillin hydrodeoxygenation (HDO) was studied in water and methanol using palladium-decorated carbon dots (Pd/CDs). The catalyst was synthesized from photo-reduction of palladium acetate using CDs as the reducing and dispersion agent, while CDs were produced via microwave treatment of glucose and urea. Pd/CDs were characterized with XRD, TEM, FT-IR, XPS, BET and ICP-OES. The selectivity to 2‑methoxy-4-methylphenol (MMP), at vanillin conversion of 100 % after 4.0 h was 98.8 % at 140 °C under 4.0 MPa of H 2 in water with 4.58 wt.% of Pd/CDs. The stability of Pd/CDs was also investigated after four times recycle under the optimal reaction conditions. CDs supported Pd reduced with NaBH 4 and hydrazine hydrate (Pd/CDs-S and Pd/CDs-H) and other carbonaceous materials (active carbon and OH functionalized multi-walled carbon nanotube) supported Pd (Pd/AC and Pd/CNTs) were also investigated for comparison. The highest selectivity to MMP achieved by Pd/CDs produced via photoreduction brings a novel use of this type of catalyst in the conversion of biomass into value-added chemicals and materials.
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Journal of Environmental Sciences
·
2023
·
IF 6.9
Xingyu Liu,Jingkun Chen,Bowen Han,Renna Li,Le Shi,Zhongbiao Wu,Xiaole Weng
Zeolites are a promising support for Pd catalysts in lean methane (CH 4 ) combustion. Herein, three types of zeolites (H-MOR, H-ZSM-5 and H-Y) were selected to estimate their structural effects and deactivation mechanisms in CH 4 combustion. We show that variations in zeolite structure and surface acidity led to distinct changes in Pd states. Pd/H-MOR with external high-dispersing Pd nanoparticles exhibited the best apparent activity, with activation energy ( E a ) at 73 kJ/mol, while Pd/H-ZSM-5 displayed the highest turnover frequency (TOF) at 19.6 × 10 −3 s −1 , presumably owing to its large particles with more step sites providing active sites in one particle for CH 4 activation. Pd/H-Y with dispersed PdO within pore channels and/or Pd 2+ ions on ion-exchange sites yielded the lowest apparent activity and TOF. Furthermore, Pd/H-MOR and Pd/H-ZSM-5 were both stable under a dry condition, but introducing 3 vol.% H 2 O caused the CH 4 conversion rate on Pd/H-MOR drop from 100% to 63% and that on Pd/H-ZSM-5 decreased remarkably from 82% to 36%. The former was shown to originate from zeolite structural dealumination, and the latter principally owed to Pd aggregation and the loss of active PdO.
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ChemCatChem
·
2023
·Vol. 15
·期 20
·e202300793
·
IF 4.5
Guoqing Wang,Miao Jiang,Zhao Sun,Leilei Qian,Guangjun Ji,Lei Ma,Cunyao Li,Hong Du,Li Yan,Yunjie Ding
Graphical A multifunctional heterogeneous Pd-POPs-CF 3 SO 3 H catalyst containing integrated acid and metal sites and anions was synthesized for tandem conversion of fructose to bio-diketones in good yield with an extraordinary TOF. Tandem conversion of biomass to value-added fine chemicals is a significant challenge. For instance, the production of fine chemicals from fructose involves conversion to 5-hydroxymethylfurfural (5-HMF), followed by another reaction and purification. Dual catalyst systems have been used in nearly every study on the tandem conversion of fructose to bio-diketones. Therefore, a sole multifunctional heterogeneous catalyst was developed in this study for the tandem conversion of fructose to bio-diketones, which has not been reported previously. Instrument corrosion and the separation or purification of 5-HMF were avoided using the multifunctional heterogeneous catalyst, which contained integrated active sites of acid, metal, and anions. The multifunctional CF 3 SO 3 H-functionalized porous-organic-polymers(POPs)-supported Pd catalyst (Pd-POPs-CF 3 SO 3 H) was prepared using a series of modifications. A bio-diketone yield of 51.0 % was achieved using Pd-POPs-CF 3 SO 3 H in the tandem conversion of fructose with an excellent TOF of 88.3 h −1 which is much more efficient than catalyst reported in literatures. Pd-POPs-CF 3 SO 3 H could be reused at least three times with stable performance. Control experiments and characterization results proved that the high specific surface area, hierarchical pore structure, abundance of CF 3 SO 3 −1 anions, and proximity of Pd moieties and acid sites (“The closer the better” principle) led to the decent performance for bio-diketone.
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RSC Advances
·
2023
·Vol. 13
·期 35
·24628-24638
·
IF 3.9
Ji-qiu Zhang,Yu-Hao Wang,Shu-jing Zhang,Yang-qian Lin,Qing-qing Guan,Xi-meng Xu
Acetylene hydrogenation is a well-accepted solution to reduce by-products in the ethylene production process, while one of the key technical difficulties lies in developing a catalyst that can provide highly dispersed active sites. In this work, a highly crystalline layered covalent organic framework (COF) material (TbBpy) with excellent thermal stability was synthesized and firstly applied as support for ultrasmall Pd nanoparticles to catalyze acetylene hydrogenation. 100% of C2H2 conversion and 88.2% of C2H4 selectivity can be obtained at 120 °C with the space velocity of 70 000 h−1. The reaction mechanism was elucidated by applying a series of characterization techniques and theoretical calculation. The results indicate that the coordination between Pd and N atom in the bipyridine functional groups of COFs successfully increased the dispersibility and stability of Pd particles, and the introduction of COFs not only improved the adsorption of acetylene and H2 onto catalyst surface, but enhanced the electron transfer process, which can be responsible for the high selectivity and activity of catalyst. This work, for the first time, reported the excellent performance of Pd@TbBpy as a catalyst for acetylene hydrogenation and will facilitate the development and application of COFs materials in the area of petrochemicals.
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高影响因子
CATALYSIS LETTERS
·
2023
·Vol. 153
·期 10
·3044-3052
·
IF 2.8
Li Kaihui,Xu Junyuan,Zhang Huan,Zhu Lihua
Abstract Cyclohexanone is a crucial intermediate for producing nylon and other industrial products. However, the direct hydrogenation of phenol for synthesizing cyclohexanone easily generates cyclohexanol and thus reduce the yield. In this work, the Pd/WO 3 catalysts with different Pd contents (Pd/WO 3 -1–0.21 wt%, Pd/WO 3 -2–0.69 wt%, Pd/WO 3 -3–2.20 wt%) are prepared via using sodium borohydride liquid phase reduction, which have good catalytic performance for phenol selective hydrogenation. The Pd/WO 3 -2 catalyst can achieve 92.9% conversion, 84.4% selectivity and high TOF (turnover frequency) of 349.1 h −1 under the reaction conditions (120 °C, 2 h, 3.0 MPa H 2 ). The nanostructures of the catalysts are extensively characterized by XRD, XPS, SEM, TEM, HRTEM, STEM and STEM-EDS elemental mapping and line-scanning. It is found that the Pd/WO 3 -2 catalyst has a high Pd dispersion and quite tiny Pd clusters. Alternatively, the stability experiment of Pd/WO 3 -2 indicates that the conversion decreases from 92.9% to 87.5% and the selectivity to cyclohexanone does not change significantly (84%) after it is recycled for five times. Graphic Abstract
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Jiaqian Ding,Xian Jiang,Caikang Wang,Zhuoya Zhu,Chang Xu,Yi Zhou,Xuan Wang,Qicheng Liu,Zhenyuan Liu,Yawen Tang,Jun Lin,Gengtao Fu
Ru with Pt-like hydrogen bond strength, knockdown cost (∼1/3 of Pt), and eximious stability is a competitive replacement for Pt-based catalysts towards the hydrogen evolution reaction (HER) in water splitting. The design of Ru-based catalysts via interface construction, crystal phase control, and specific light element doping to realize the impressive promotion of limited activity and stability remains challenging. Herein, we report the fabrication of Pd@RuP core-shell nanorods (NRs) via an epitaxial growth method, where ultrathin RuP shells extend the face-centered cubic ( fcc ) crystal structure and (111) plane of the Pd NRs core. Density functional theory results confirm that the core-shell interface engineering and P doping synergistically accelerate electron transfer and moderate the d -band center to generate a suitable affinity for H*, thus optimizing HER kinetics. Compared with Pd@Ru NRs and Pt/C, the Pd@RuP NRs exhibit preferable electrocatalytic stability and superior activity with a low overpotential of 18 mV at 10 mA cm −2 in the alkaline HER process. Furthermore, the integrated Pd@RuP//RuO 2 -based electrolyzer also displays a low operation potential of 1.42 V to acquire 10 mA cm −2 , demonstrating great potential for practical water electrolysis. Our work presents an efficient avenue to design Ru-based electrocatalysts via epitaxial growth for extraordinary HER performance.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Di Wang,Hongcen Yang,Shuhao Tian,Guo Liu,Ying Wang,Xiao Sun,Zhixia Wang,Juan Hou,Fei Ma,Shanglong Peng
Hydrogen energy is regarded as the clean energy alternative for fossil energy. Hydrogen evolution reaction (HER) is a sustainable way for the production of hydrogen energy. However, commercial platinum (Pt) catalysts for HER are expensive and scarce, which will not fully meet the demand of the future market. Therefore, scientists have been actively exploring alternatives to Pt-based catalysts. Studies have shown that palladium (Pd) and Pt have similar catalytic activity in HER. Small molecular Pd nanoclusters can be used as a perfect HER activity center. Herein, anchoring of Pd nanoclusters (Pd NCs) on sulfur-vacancy-enriched ZnIn 2 S 4 nanosheets (Pd/ZIS-T) has been successfully achieved. The zeta potential value for ZnIn 2 S 4 is −59.9 mV, indicating that the surface of ZnIn 2 S 4 is abundant negatively charged in deionized water, thus providing plentiful anchoring sites to absorb Pd 2+ . The results show that the synergistic effect of Pd NCs and sulfur vacancies will endow the obtained catalyst with excellent electrocatalytic activity and stability. It also managed to reducing costs by reducing noble metal content. In particular, the Pd/ZIS-T electrocatalyst with excellent performance delivered low overpotential of 25 mV at 10 mA cm −2 and small Tafel slope of 33 mV dec -1 in acidic electrolyte.
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Asian Journal of Organic Chemistry
·
2023
·Vol. 12
·期 7
·e202300216
·
IF 2.7
Yi-Ying Zhuang,Xiao-Chao Chen,Kai-Chun Zhao,Guo-Sheng Zhang,Yu-Fen Xie,Yong Lu,Ye Liu
Graphical Pd-catalyzed anti -Markovnikov hydrocarboxylation of vinylarenes with formic acid free of auxiliary additive has been reported. This work was financially supported by the National Natural Science Foundation of China (Nos. 22172052 and 21972045), and the Research Funds of Happiness Flower ECNU (2022ST2203).
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 19
·10222-10227
·
IF 11.9
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Kai Deng,Hongjie Yu,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Water electrolysis for hydrogen production consumes abundant electronic energy owing to the sluggish oxygen evolution reaction (OER), so the integration of the hydrogen evolution reaction (HER) with thermodynamically more favorable oxidation reactions is a promising strategy for energy-efficient hydrogen production. Herein, we propose the epitaxial confinement of rhodium nanoparticles (NPs) to palladium metallene (Rh/Pd metallene) for hydrogen production assisted by the hydrazine oxidation reaction (HzOR). The two-dimensional structure of Rh/Pd metallene provides sufficient active sites as well as a rapid charge transfer rate. The interface of Pd metallene with Rh NPs ensembles to modulate the electronic state, thus optimizing the adsorption energy of reaction intermediates. The Rh/Pd metallene exhibits splendid HER and HzOR activities, with overpotentials of 59 and 7 mV at 10 mA cm−2, respectively. In the two-electrode construction of a hydrazine oxidation-assisted water splitting system, the Rh/Pd metallene only needs a low overpotential of 0.19 V to produce hydrogen at a current density of 100 mA cm−2. This research offers a viable approach for designing nanosheet/nanoparticle heterojunction as an attractive modular platform for energy-saving hydrogen production.
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