RENEWABLE ENERGY
·
2022
·
IF 8.634
Siteng Rong,Hongzi Tan,Zhaobin Pang,Zhiyuan Zong,Rongrong Zhao,Zhihe Li,Zhe-Ning Chen,Ning-Ning Zhang,Weiming Yi,Hongyou Cui
Lignin could be depolymerized into large amount of phenolic compounds via fast pyrolysis . The upgrade of phenolic compounds via hydrodeoxygenation (HDO) involves multiple reaction pathways. It is challenging to selectively remove the oxygen-containing groups while keeping the aromatic rings intact. In this work, hierarchical Nb 2 O 5 (H–Nb 2 O 5 ) microspheres with abundant oxygen vacancies were synthesized to anchor the Pd clusters, which is featured with strong metal-support interaction via the electron transfer between Pd species and Nb species. For phenol HDO reaction, the oxygen vacancies were prone to interact with the phenolic hydroxy groups, resulting in phenol molecule adsorbed in a “nonplanar” manner, greatly weakening the C Ar -O bonds and averting the ring hydrogenation. Besides, the activated hydrogen atoms on Pd clusters could migrate to the vicinity of oxygen vacancies via spillover, promoting the cleavage of C Ar -O bond to obtain benzene. Current work provides a deep insight into the synergetic catalytic mechanism of Pd/H–Nb 2 O 5 catalyst for phenol HDO reaction, and also sheds light on the design and synthesis of high-efficient catalysts in other heterogeneous catalysis fields.
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高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 152
·期 11
·3437-3446
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IF 2.936
Yue Yihang,Li Yong,Wang Tingting,Wang Shifeng,Han Lin,Du Chun
A Pd/CeO 2 -M with high methanol oxidation performance was prepared from metal–organic framework (MOF). The reaction results indicate that the Pd/CeO 2 -M could achieve 100% methanol oxidation at 200 °C over the traditional Pd/CeO 2 -C at 350 °C. The high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and Raman show that the Pd was uniformly distributed over the CeO 2 that was rich in oxygen vacancies. The methanol temperature program surface reaction (MeOH-TPSR) demonstrates that the Pd/CeO 2 -M could effectively decompose methanol at a lower temperature with the assistance of oxygen vacancies compared with Pd/CeO 2 -C. Methanol oxidation was conducted with in-situ Raman, CO diffuse reflectance infrared Fourier transformed spectroscopy (CO-DRIFTS) and in-situ DRIFTS to elucidate the reaction mechanism and establish the structure–activity relationship. The oxygen vacancies have participated in the assistance of methanol oxidation, which was revealed via in-situ Raman. The CO-DRIFTS indicates that the chemisorbed CO was more in linear form, which demonstrates that the Pd particles were over CeO 2 -M with a smaller size. The in-situ DRIFTS experiments show the methanol could be further effectively oxidized to bidentate formate over Pd/CeO 2 -M with the assistance of oxygen vacancies. The Pd/CeO 2 -M catalysis and its enhancement mechanism studies provided a potential strategy in the VOC removal catalysis development. Graphical Abstract
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 12
·2028-2037
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IF 7.571
Chen Yang,Wenli Jiang,Yongqi Yu,Hui Zhang,Chenxin Cai,Qingming Shen
The integration of photothermal therapy (PTT) and photodynamic therapy (PDT) has become a promising cancer treatment method. Herein, anisotropic metal hetero-nanostructure Pd-tipped Au nanorods (PTA NRs) were fabricated, which exhibit plasmon-enhanced photothermal performance under near-infrared laser irradiation. Due to their anisotropic nanostructure, PTA NRs promote the generation of energetic hot electrons and prolong the separation time of electrons and holes. The hot electrons could generate heat energy through the electron–phonon relaxation process and produce reactive oxygen species through energy and electron transformation processes. Because of their high NIR absorption cross-section, as well as good photostability, PTA NRs can be used for NIR-activated photoacoustic imaging-guided PTT-PDT combination cancer therapy. Experiments in tumor-bearing mice proved that PTA NRs exhibit excellent anti-tumor effects, with little side effects on normal organs, making them promising for NIR cancer phototherapy.
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PubMed
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
De Ping Chen,Lei Yuan,Meng Jue Li,Wen Jing Han,Xu Dong Liu,Xi Chuan Liu,Chao Yang Wang
Pd is a highly active non-Pt anode in direct ethanol fuel cells, and its morphology and structural composition heavily influence its electrocatalytic efficiency. In this study, three-dimensional (3D)-hollow Au microspheres (HNPs-Au) as a support for the Pd monolayer (HNPs-Au@Pd) were synthesized using a simple template method and galvanic replacement reaction. The experimental results and theoretical calculations show that the presence of HNPs-Au enhances the catalytic activity of ethanol oxidation in alkaline media, improving the electroactivity of metallic Pd. Benefiting from the 3D-hollow-porous structure and the significant synergistic impact between Au and Pd (balancing the adsorption energy of the intermediate and reactant molecules), HNPs-Au@Pd achieves a 10.8-fold mass activity and a 3.3-fold enhancement of the specific activity for the ethanol oxidation reaction when compared to commercial Pd/C. The present work not only enriches the preparation strategy of porous metal materials but also opens up a sector for the construction of anodic electrocatalysts with a wide range of applications.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8855-8862
·
IF 3.925
Yabing Tian,Chen Xing,Wenxiang Wang,Shiguo Zhang,Yan Zhang
Pd-catalyzed Suzuki–Miyaura cross-coupling reactions have attracted considerable attention. Porous organic polymers (POPs) are potential heterogeneous catalysts to overcome the shortcomings of the homogeneous reaction. However, most POPs are microporous, which strongly hindered the mass transfer process during the catalytic reaction. In this work, a Pd-containing, highly crosslinked, mesoporous poly(ionic liquid) (SMPIL–Pd) was designed as a heterogeneous catalyst for efficient Suzuki–Miyaura coupling reactions. This catalyst was fabricated by hyper-crosslinking of a salen-containing mesoporous poly(ionic liquid) via a simple Friedel–Crafts alkylation reaction followed by Pd(II) coordination via the –N2O2– tetradentate structure of the salen structure. A series of characterization studies revealed that SMPIL–Pd possesses predominant porosity and extremely rigid networks, highly dispersed catalytic active sites, mesoporous structures, and large specific surface areas. Consequently, this catalyst exhibited excellent catalytic activity towards Suzuki–Miyaura coupling reactions under an air atmosphere in 50% aqueous ethanol. SMPIL–Pd also demonstrated outstanding stability and recyclability, and it can be reused seven cycles without a significant loss of activity.
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APPLIED CLAY SCIENCE
·
2022
·
IF 5.907
Xuemin Zhong,Yanfu Wei,Samahe Sadjadi,Dong Liu,Mengyuan Li,Ting Yu,Guanzheng Zhuang,Peng Yuan
Aerobic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2, 5-furandicarboxylic acid (FDCA) is an important reaction for producing green and sustainable chemicals. Herein, natural clay mineral palygorskite (Pal)-supported bimetallic Pt–Pd catalyst for the oxidation of HMF to FDCA in water without the addition of any bases was developed. The 1Pt 9 Pd 1 /Pal catalyst with Pt/Pd molar ratio of 9/1 exhibited excellent catalytic performance, and 100% HMF conversion and 99% FDCA yield were obtained under optimum reaction conditions after 12 h, which was mainly attributed to the synergy between palygorskite and bimetallic Pt–Pd nanoparticles . Palygorskite used as support realized the immobilization and dispersion of bimetallic nanoparticles, increasing the catalytic activity . The basicity of palygorskite and alloying effects between Pt and Pd facilitated the formation of FDCA by synergistically catalyzing the oxidation of alcohol and aldehyde groups in the reactants and intermediates. Furthermore, this catalyst showed good stability and reusability . The present work provides a highly efficient, cost-effective, and environmentally benign catalyst for the base-free oxidation of HMF to FDCA in practical industrial applications.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xiaolu Sun,Lifeng Hao,Liuyang Chen,Xingkui Guo,Chuang Han,Jingfu Chen,Weicheng Jiao,Rongguo Wang,Xiaodong He
Here, we demonstrate a rapidly responsive colorimetric hydrogen detector based on Pd/MoO 3 nanocomposites for hydrogen leakage monitoring at room temperature. The Mo 5+ -rich MoO 3 nanobelts are synthesized via a simple one-step hydrothermal method by adding NaCl as the mineralizer. The structure of the detector is fabricated by a general spray deposition technique, not only forming uniform porous microstructures to promote the adsorption and diffusion of H 2 but also solving the issue of performance degradation in ambient conditions by the strategy of on-site fabrication for immediate detection. The detector exhibits a rapid color change which could be recognized with naked eyes within 10 s even in as low as 1% of H 2 at room temperature (25 °C) owing to the high content of active absorption sites (Mo 5+ ) and the large surface area. The detector is also tested on a hydrogen storage tank with a prefabricated defect in the inner liner and exhibits a prompt and intense color change at the exact hydrogen leakage site, demonstrating its high efficiency in the visual hydrogen leakage detection in complicated systems. The facile fabrication approach as well as the rapid visual detection strategy enable the detector extensively applicable in the hydrogen industry.
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高影响因子
JACS Au
·
2022
·
IF 0
Yuhai Sun,Junliang Wu,Yaolin Wang,Jingjing Li,Ni Wang,Jonathan Harding,Shengpeng Mo,Limin Chen,Peirong Chen,Mingli Fu,Daiqi Ye,Jun Huang,Xin Tu
Plasma-catalytic CO2 hydrogenation is a complex chemical process combining plasma-assisted gas-phase and surface reactions. Herein, we investigated CO2 hydrogenation over Pd/ZnO and ZnO in a tubular dielectric barrier discharge (DBD) reactor at ambient pressure. Compared to the CO2 hydrogenation using Plasma Only or Plasma + ZnO, placing Pd/ZnO in the DBD almost doubled the conversion of CO2 (36.7%) and CO yield (35.5%). The reaction pathways in the plasma-enhanced catalytic hydrogenation of CO2 were investigated by in situ Fourier transform infrared (FTIR) spectroscopy using a novel integrated in situ DBD/FTIR gas cell reactor, combined with online mass spectrometry (MS) analysis, kinetic analysis, and emission spectroscopic measurements. In plasma CO2 hydrogenation over Pd/ZnO, the hydrogenation of adsorbed surface CO2 on Pd/ZnO is the dominant reaction route for the enhanced CO2 conversion, which can be ascribed to the generation of a ZnOx overlay as a result of the strong metal–support interactions (SMSI) at the Pd–ZnO interface and the presence of abundant H species at the surface of Pd/ZnO; however, this important surface reaction can be limited in the Plasma + ZnO system due to a lack of active H species present on the ZnO surface and the absence of the SMSI. Instead, CO2 splitting to CO, both in the plasma gas phase and on the surface of ZnO, is believed to make an important contribution to the conversion of CO2 in the Plasma + ZnO system.
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PubMed
CATALYSIS TODAY
·
2022
·
IF 6.562
Peng Bai,Tao Zhou,Xiaohua Wang,Xiaofei Liu,Yi Wang,Yue Wang,Edgar Muhumuza,Yonghui Zhang,Pingping Wu
A series of γ-Al 2 O 3 supported gold-palladium (Au-Pd) alloy nanoparticles (NPs) catalysts were synthesized by a one-pot approach applying mercapto-propyl-trimethoxysilane (MPTMS) as an anchoring ligand. Homogeneously dispersed Au-Pd alloy NPs were observed on the prepared catalysts and their catalytic performance in benzyl alcohol partial oxidation was investigated. Results showed that the highest benzaldehyde yield was achieved on catalyst Au-Pd/7%MPTMS-γ-Al 2 O 3 with a benzaldehyde selectivity of 90%. By establishing the structure-performance relationship, the high activity of catalysts with MPTMS modification was attributed to the anchoring and dispersion effect of MPTMS on Au-Pd NPs, while the high benzaldehyde selectivity was due to the formation of more surface Lewis acid sites after introducing MPTMS, protecting the benzaldehyde from over-oxidation to byproducts.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Qiqi Lu,Xiu-Zhi Wei,Jianguo Liu,Longlong Ma
Zeolite-tailored encapsulation of metal nanoparticles exhibits prominent catalytic performance in many fields especially for selective hydrogenation reaction due to the modulation effect of the zeolite microenvironment. Here, Pd nanoparticles encapsulated in MFI zeolite by an in-situ encapsulation method were first used in the selective hydrogenation of nitrile into a primary amine. After introducing KOH for mediating the acid-base property of zeolite microenvironment, the as-synthesized [email protected] manifested an improved selectivity in the synthesis of primary amine from nitrile, while outperformed both commercial catalysts and conventional Pd supported on zeolite catalyst. The remarkable performance of [email protected] could be attributed to both the basic property of the S-1-K zeolite for inhibiting the side reactions and the highly dispersed and ultrasmall Pd clusters for superior catalytic activity. Besides, the best yield of 81% was achieved at 80 °C, 5 bar H 2 , 2 h in ammonia solution via optimization experiments, and the moderate applicability of [email protected] catalyst was obtained by substrate scope test.
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高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Xiaoda Niu,Shuang Liu,Yong Men,Lin Li,Liangmin Xiong,Kailiang Guo,Junzhe Xu,Kunfeng Zhao,Ya Li,Wei An,Jinguo Wang
Hydrogenation of quinones is an efficient way to produce hydroquinone compounds. Typically, 2,3,5-trimethylhydroquinone (TMHQ), the key intermediate of vitamin E, can be produced via hydrogenation of 2,3,5-trimethylbenzoquinone (TMBQ). In order to effectively obtain the target products, the exploration of efficient heterogeneous catalysts is highly desired. In this study, supported Pd nanocluster catalysts (PdN/TiVo) were designed through a deposition-precipitation method over TiO 2 support with surface defects (TiVo) to achieve high atomic utilization efficiency of the noble metal Pd under mild reaction conditions. The characterization showed that oxygen vacancies generated by H 2 reduction on the support TiO 2 acted as specific sites to promote the formation of the coupled eutectic growth structure composed of the active metal Pd and TiVo. The active metal Pd which not only exhibited high dispersion but also formed electron-rich active sites can activate H 2 while the Ti 3+ atoms at oxygen vacancy sites can adsorb the oxygen species from TMBQ, thereby a synergistic catalytic effect can be shown to enhance the adsorption and hydrogenation of C=O bonds. Thus PdN/TiVo revealed a high yield of TMHQ of 96% and TOF of 276 min −1 under a considerably wild condition (45°C, 0.2 MPa, 60 min). By comparison, state-of-the-art carbon based Pd catalysts (PdN/C) acquired only 29% yield and 41 min −1 TOF in the same way. The simultaneous engineering of Pd catalyst and oxygen vacancies on TiO 2 offers a new strategy to develop efficient heterogeneous catalysts for hydrogenation of quinones.
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Nature Biomedical Engineering
·
2021
·Vol. 6
·期 1
·32-43
·
IF 25.671
Zheng Di-Wei,Deng Wei-Wei,Song Wen-Fang,Wu Cong-Cong,Liu Jie,Hong Sheng,Zhuang Ze-Nan,Cheng Han,Sun Zhi-Jun,Zhang Xian-Zheng
Because a host’s immune system is affected by host–microbiota interactions, means of modulating the microbiota could be leveraged to augment the effectiveness of cancer therapies. Here we report that patients with oral squamous cell carcinoma (OSCC) whose tumours contained higher levels of bacteria of the genus Peptostreptococcus had higher probability of long-term survival. We then show that in mice with murine OSCC tumours injected with oral microbiota from patients with OSCCs, antitumour responses were enhanced by the subcutaneous delivery of an adhesive hydrogel incorporating silver nanoparticles (which inhibited the growth of bacteria competing with Peptostreptococcus ) alongside the intratumoural delivery of the bacterium P. anaerobius (which upregulated the levels of Peptostreptococcus ). We also show that in mice with subcutaneous or orthotopic murine OSCC tumours, combination therapy with the two components (nanoparticle-incorporating hydrogel and exogenous P. anaerobius ) synergized with checkpoint inhibition with programmed death-1. Our findings suggest that biomaterials can be designed to modulate human microbiota to augment antitumour immune responses.
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高影响因子
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