JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 24
·10482-10491
·
IF 3.553
She Tiantian,Niu Libo,Nie Shilin,Li Huafan,Qiao Xianliang,Ma Yuanyuan,Han Xue,Chen Guofeng,Bai Guoyi
A novel sodium alginate-based Pd-3D double network hydrogel Pd/Ca–Alg–PAAS has been fabricated and successfully applied in the selective hydrogenation of phenol for the first time. The prepared catalyst showed excellent catalytic activity and high selectivity (99.8%) for cyclohexanone in the selective hydrogenation of phenol. Furthermore, this double network hydrogel of Pd/Ca–Alg–PAAS still kept a conversion of over 80% with the selectivity for cyclohexanone being over 99% after 6 runs, superior to the single network hydrogel of Pd/Ca–Alg. TEM and FT-IR results demonstrated that the Pd species were highly dispersed in Pd/Ca–Alg–PAAS, and the addition of sodium polyacrylate could enhance the interaction between hydrogel and Pd 2+ and thus inhibit the agglomeration and loss of the active Pd species, accounting for the good stability of Pd/Ca–Alg–PAAS.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Cong Luo,Jianghua Yang,Jinling Li,Shijie He,Bowen Meng,Tao Shao,Qiankun Zhang,Dongxia Zhang,Xibin Zhou
A strategy for the synthesis of Au@N-CQDs@Pd three-layer core-shell nanoparticles without the use of any surfactant is proposed in this work. Herein, N-doped carbon quantum dots (N-CQDs) are used as the reducing agent, stabilizing agent, and shape-directing agent. The morphology and structure of the final product were characterized by Transmission electron microscopy (TEM), high-resolution TEM (HRTEM), and X-ray powder diffraction (XRD). The electrocatalytic test indicates the as-synthesized Au@N-CQDs@Pd 20 exhibites excellent activity for methanol oxidation in alkaline media, which is approximately 6 times higher than commercial Pd/C. And its resistance to CO and stability are also greatly improved. This work provides a simple and straightforward approach to prepare bimetallic core-shell electrocatalyst by using CQDs with high catalytic activity for alkaline fuel cells .
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GREEN CHEMISTRY
·
2020
·Vol. 22
·期 13
·4341-4349
·
IF 9.48
Yuxue Xiao,Qingwei Meng,Xiaoli Pan,Chao Zhang,Zaihui Fu,Changzhi Li
para-Xylene (PX) is a basic building block of polyethylene terephthalate, which is currently produced from petroleum resources. Developing a renewable route to PX is highly desirable to address both economic and environmental concerns. Several attempts used noble metal catalysts, e.g. Pd/Al2O3, to synthesize PX from biomass-derived 4-methyl-3-cyclohexene-1-carboxaldehyde (4-MCHCA), but suffered from a severe decarbonylation reaction, resulting in toluene as the main product. In this paper, we report an FeOx modification strategy to suppress the decarbonylation reaction on a Pd/Al2O3 catalyst, leading to a drastic shift in selectivity towards PX with a yield up to 81% via a cascade dehydroaromatization–hydrodeoxygenation (DHA–HDO) pathway. Characterization and control experiments revealed that the electron density of Pd sites decreased in an FeOx-modified Pd/Al2O3 catalyst compared to Pd/Al2O3, thus tuning the preferential adsorption mode of the substrate from η2-(C,O), the key transition state of the decarbonylation reaction, to the η1-(O) mode that favors the hydrodeoxygenation process. Notably, this designed catalyst is highly stable and is readily applicable in the selective synthesis of a broad range of desired aromatic chemicals via the same DHA–HDO pathway from cyclohex-3-enecarbaldehyde derivatives. Overall, this work develops a controllable catalyst modification strategy that tailors an efficient catalyst for petroleum-independent bio-PX synthesis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qianying Fang,Zhicheng Jiang,Kai Guo,Xudong Liu,Zheng Li,Guiying Li,Changwei Hu
Two-step conversion of pubescens to aromatic monomers and small molecular weight oligomers (mainly dimers and trimers) was studied. Lignin-derived oligomers (LDO) were obtained by formic acid assisted solvo-thermal conversion of pubescens in the H 2 O-ethanol system at 160 ℃. In the second step, hydrogenolysis of LDO on Pd/NbOPO 4 catalyst was carried out over the temperature range of 60–120 ℃. Pd/NbOPO 4 showed acceptable catalytic performance for efficient degradation of oligomers at low temperature. The NbO x species on the catalyst facilitated the breakage of C O C bonds to depolymerize the oligomers toward small molecules, while Pd species accelerated the selective hydrogenation of side chain and furans. The esterification of S (Syringol) unit phenols took place simultaneously with the depolymerization of LDO. The hydrogenated mixture at 100 ℃ and reaction time of 20 h had an average molecular weight of 908 g/mol, and the yield of aromatic monomers was 22.4 wt.% based on lignin contained.
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CERAMICS INTERNATIONAL
·
2019
·
IF 3.45
Kelin Hu,Feipeng Wang,Hongcheng Liu,Yanqiong Li,Wen Zeng
Pd-doped SnO 2 nanofibres were prepared by electrospinning and magnetron sputtering . It was found that the efficiency of gas sensing properties in these fibres depends primarily on the density of oxygen vacancies , which can be regulated by plasma treatment. We demonstrated that moderate plasma treatment can increase the oxygen vacancy as well as improve the gas sensing performance of SnO 2. However, excessive plasma treatment led to the production of other substances that deteriorated the gas sensing performance. Furthermore, the best results for hydrogen gas sensing were obtained when the nanofibres were subjected to plasma treatment for 1 min. The fabricated material demonstrated a response of more than 53 for 500 ppm hydrogen at the optimum temperature (130 °C), which is a significant improvement as compared to sensors without plasma treatment. Evidently, plasma treatment is an effective method to further enhance the sensing properties of the fabricated nanofibres.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Li Yongfeng,Liao Qianyan,Ling Weizhao,Ye Fan,Liu Fangfang,Zhang Xipeng,He Jiajun,Cheng Gao
Exploring high-efficiency and stable monolithic structured catalysts is vital for catalytic combustion of volatile organic compounds. Herein, we prepared a series of Pd/δ-MnO2 nanoflower arrays monolithic integrated catalysts (0.01–0.07 wt% theoretical Pd loading) via the hydrothermal growth of δ-MnO2 nanoflowers onto the honeycomb cordierite, which subsequently served as the carrier for loading the Pd nanoparticles (NPs) through the electroless plating route. Moreover, we characterized the resulting monolithic integrated catalysts in detail and evaluated their catalytic activities for toluene combustion, in comparison to the controlled samples including only Pd NPs loading and the δ-MnO2 nanoflower arrays. Amongst all the monolithic samples, the Pd/δ-MnO2 nanoflower arrays monolithic catalyst with 0.05 wt% theoretical Pd loading delivered the best catalytic performance, reaching 90% toluene conversion at 221°C at a gas hourly space velocity (GHSV) of 10,000 h−1. Moreover, this sample displayed superior catalytic activity for o-xylene combustion under a GHSV of 10,000 h−1. The monolithic sample with optimal catalytic activity also displayed excellent catalytic stability after 30 h constant reaction at 210 and 221°C.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Ruifa Su,Qianqian Han,Cheng Xu,Junchen Ouyang,Fanchen Meng,Yingyu Zhou,Xinglong Zhang,Zhida Gu,Weina Zhang,Fengwei Huo,Suoying Zhang
Pd/C catalysts have been widely applied in the debenzylation process due to their excellent ability of hydrogenolysis. However, they have been suffering from the problems of agglomeration and loss of active components, which lead to decreased and unstable activity. Thus, it is still a challenge to achieve Pd/C catalysts with high activity and stability. Herein, we propose a strategy for preparing Pd/C catalysts on porous carbon hollow spheres by a microwave discharge method. Due to the high-temperature property and reducibility of microwave discharge, Pd precursors can be rapidly reduced, resulting in well-dispersed Pd nanoparticles with a small size on the carbon carrier. Besides, the matched mesopores in the carbon hollow spheres can anchor Pd nanoparticles and effectively reduce the agglomeration and loss of Pd nanoparticles during the catalytic reaction. As a result, the as-prepared Pd/mesoporous carbon hollow spheres exhibit high and stable activity in the debenzylation reaction.
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ACS Catalysis
·
2026
·
IF 13.6
Xiao Jing,Shen Meiqing,Shen Gurong,Li Xinhua,Jia Liwei,Wang Yilin,Li Wei,Gao Feng
Developing Pd-based catalysts for methane oxidation that combine low-temperature activity with strong water tolerance remains a major challenge for emission control applications. Herein, we introduce a high-entropy architecture into Co 3 O 4 -based spinel supports to regulate Pd-support interfacial interactions. The resulting high-entropy support (HE-Co-Sp) forms a hybridized and electronically delocalized Co–O–M (M = multiple cations) network, providing dynamic electron-buffering capability. This electronic framework promotes rapid replenishment of reactive oxygen species at Pd sites, thereby enhancing low-temperature methane oxidation activity. Concurrently, interfacial electronic coupling induces electron transfer from the support to Pd, as evidenced by XANES, EXAFS, and Pd 3d XPS measurements, leading to a moderated Pd electronic state and suppressed H 2 O adsorption. As a result, Pd/HE-Co-Sp exhibits markedly improved stability under wet methane oxidation under highly O 2 -rich conditions compared with Pd/θ-Al 2 O 3 , Pd/Co 3 O 4 , and Pd/MnCo 2 O 4 . These findings establish high-entropy-induced electronic delocalization as an effective strategy for designing water-tolerant methane oxidation catalysts.
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Molecular Catalysis
·
2023
·
IF 4.6
Yanzhao Gao,Xianglei Meng,Shiqi Huang,Hui Wu,Liantao Jiang,Yu Zhou,Yuting Song,Yanyan Diao
Gamma alumina is widely utilized for preparing the supported noble metal catalysts for the hydrogenation reaction. It is an effective strategy to improve the catalytic performance of catalysts via modifying gamma alumina with alkaline earth metal to regulate its surface acidity and electronic properties. Herein, Pd catalysts supported by Al 2 O 3 and Mg-modified Al 2 O 3 are synthesized via the wet impregnation method, and the effects of MgO doping on the structure, composition, and surface acidity of Pd/γ-Al 2 O 3 catalysts are investigated via X-ray diffraction patterns (XRD), Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and Temperature programmed desorption (TPD). The results show that Pd/MgO-Al 2 O 3 –2 (γ-Al 2 O 3 modified with 2 wt% Mg) has more metallic state palladium and weak acid sites and exhibits the best catalytic performance for the hydrogenation of perfluoro-4-methyl-2-pentene (D1). Density functional theory (DFT) calculations on Pd/Al 2 O 3 and Pd/MgO-Al 2 O 3 –2 catalysts are also performed to further explore the mechanism of D1 hydrogenation. The studies for Gibbs free energy of the potential reaction steps and intermediates reveal a complex process to generate the target product C 6 F 12 H 2 , and the rate-determining-step is the addition of the first hydrogen on the second carbon of perfluoro-4-methyl-2-pentene molecule.
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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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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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