Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Juan Miao,Jingmin Wang,Zhen Lv,Xiaoying Feng,Ning Zhang,Xinquan Zhou,Hang Xu,Xuefeng Wei,Shuge Peng
A nitrogen-doped carbon-anchored single atom Pd (SA-Pd/NC) electrocatalyst was prepared by pyrolysis of Pd-doped zeolite imidazolite framework (ZIF) precursors. The SA-Pd/NC catalyst was characterized by high-resolution transmission electron microscopy , aberration-corrected high-angle annular dark field scanning transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and Raman spectrometry and applied in the degradation of 2,4-dichlorophenol (2,4-DCP). We demonstrate that the SA-Pd/NC catalyst has dual functions, with both electrocatalytic hydrodechlorination (ECH) activity and in situ heterogeneous electro-Fenton (hetero-EF) activity even at low current density. The ECH process was the main pathway of 2,4-DCP degradation without oxygen aeration. Under aerobic conditions , hetero-EF coupling with ECH occurred simultaneously on the SA-Pd/NC cathode, i.e., the dechlorination product phenol was oxidatively degraded with the reactive oxygen species produced on the electrode. The degradation rate of 2,4-DCP and TOC removal rate reached 95.1% and 37.6%, respectively, with a current density of 2.5 mA cm −2 and an initial pH of 3.0. This work provides the design of bifunctional single-atom catalysts for 2,4-DCP degradation, including dechlorination and mineralization.
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RSC Advances
·
2023
·Vol. 13
·期 39
·27283-27291
·
IF 3.9
Ying Shen,Hongyuan Wu,Xia Luo,Haizhi Zhang,Liming Cheng
In addition to size, shape and morphology, enzyme–mimetic property could be efficiently regulated by controlling composition, forming complexes or hybrids, and surface modification. Herein, Pd nanoparticles with an average diameter of 2.52 nm were decorated on ultrathin 2D copper(II)-porphyrin derived metal–organic framework (MOF) nanosheets by a simple reduction method for catalytic activity regulation. In comparison with other nanozymes, the as-synthesized Pd modified 2D MOF hybrid nanosheets (Pd@Cu-TCPP(Fe)) presented excellent peroxidase–mimic activity, exhibiting an even superior catalytic ability towards H2O2 with a Michaelis–Menten constant as low as 2.33 mM. Based on a cascade reaction between glucose oxidase and Pd@Cu-TCPP(Fe), a colorimetric method for the detection of glucose was established and validated with a wide linear range (0.2–8.0 mM), good recovery (89.5–94.2%) and nice reproducibility (3.65%). All these features guaranteed its excellent ability for glucose determination in human cerebrospinal fluids. This study could offer a valuable reference for constructing novel optical biosensors.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Qingqing Wu,Jiaorong Yan,Mingxiang Jiang,Qiguang Dai,Jinyan Wu,Minh Ngoc Ha,Qingping Ke,Xingyi Wang,Wangcheng Zhan
Two-dimensional γ-Al 2 O 3 nanosheet with rich pentacoordinate Al 3+ sites which can nicely stabilize noble metals via strong interactions between metal and support has been focused. However, the synthesis of ultrathin and highly thermal-stable Al 2 O 3 is challenging. Herein, we report an effective approach to synthesize ultrathin Al 2 O 3 nanosheets with regular leaf-like architecture as well as high thermal-stability. A novel intercalation-swelling-exfoliation pathway was proposed to elucidate the formation of ultrathin sheet-like structure and then its morphology/thickness could be further adjusted via a dissolution-growth induced by phosphate. Meanwhile, the presence of phosphate further enhanced thermal stability of Al 2 O 3 nanosheets due to the occupation or depletion of high-reactive sites and surface hydroxy groups. Subsequently, the thermally stable γ-Al 2 O 3 nanosheets with moderate anchoring sites was used as a support of Pd and investigated for catalytic combustion of propane. The Pd/Al 2 O 3 nanosheet exhibited a superior catalytic activity for propane combustion and the complete conversion was below 300 °C, more importantly, the outstanding resistance to high temperature (1000 °C) was observed, which was ascribed to the re-dispersion of Pd particles and the occurrence of strong metal-support interaction (SMSI) at high temperature.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Qiang Zhao,Chiheng Chu,Xin Xiao,Baoliang Chen
The precisely coupling of metal nanoparticles with support domain are crucial to enhance the catalytic activity and stability of supported metal nanoparticle catalysts (MNPs). Here we selectively anchor Pd nanoparticles to the sp 2 domain in graphene-based aerogel constructed with base-washed graphene oxide (BGO) by removing oxidative debris (OD). The effects of OD on the size and chemical composition of Pd nanoparticles in aerogels are initially unveiled. The removal of OD nanoparticles prompt selective coupling of Pd nanoparticles to the exposed sp 2 -hybridized domain on BGO nanosheets, and then prevent it from agglomeration. As a result, the Pd nanoparticle size of self-assembled Pd/BGA is 4.67 times smaller than that of traditional Pd/graphene oxide aerogel (Pd/GA). The optimal catalytic activity of Pd/BGA for the model catalytic reduction of 4-nitrophenol is 15 times higher than that of Pd/GA. Pd/BGA could maintain its superior catalytic activity and achieves 98.72% conversion in the fifth cycle. The superior catalytic performance could be ascribed to the small Pd nanoparticles and high percentage of Pd(0) in Pd/BGA, and the enhanced electronic conductivity of Pd/BGA. These integrated merits of Pd/BGA as heterogeneous catalysts are attributed to selectively anchor Pd nanoparticles on sp 2 -hybridized domain of graphene-based aerogel, and strongly coupled interaction of MNPs with support. The structure-regulated BGO nanosheets could serve as versatile building blocks for fabricating MNPs/graphene aerogels with superior performance for catalytic transformation of water pollutants .
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JOURNAL OF WOOD CHEMISTRY AND TECHNOLOGY
·
2021
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IF 2.63
Dong Chen,Rongrong Miao,Liang He,Qingqing Guan
Ethyne is often an unwanted impurity in ethene streams used in plastics industry. Supported Pd catalysts offer high ethyne conversion, but poor ethene selectivity due to over-hydrogenation which leads to the formation of carbonaceous deposits. In this paper, acrylamide was grafted by free radical polymerization onto bagasse pith hemicellulose (to form HEMI-g-AAMs), which was then used as a porous bio-based carrier of Pd nanoparticles. The obtained Pd/HEMI-g-AAMs catalyst showed an ethyne conversion and ethene selectivity of 100% and 94.70%, respectively, at 100 °C and a space velocity of 70,000 h−1. The nitrogen-rich bio-based support regulated the physicochemical properties and catalytic activity of the supported Pd nanoparticles. Results guide the development of new and improved Pd-based catalysts for the partial catalytic hydrogenation of ethyne to ethene.
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Solar RRL
·
2021
·Vol. 5
·期 4
·2000813
·
IF 8.582
Di Li,Changjian Zhou,Zhongkai Xie,Donghai Chen,Yimeng Zhou,Xiangli Shi,Deli Jiang,Min Chen,Weidong Shi
Due to the low charge separation efficiency and high stability of the CO 2 molecule, photoreduction of CO 2 into a single multielectron product such as CH 4 with a simultaneous high conversion rate and selectivity is challenging. Therefore, it is highly desirable to accelerate charge separation and transfer and provide an electron-enriched catalyst surface for the deep reduction of CO 2 . Herein, a Pd/Cu 2 O/TiO 2 ternary hybrid photocatalyst consisting of Pd nanoparticles (NPs) and Cu 2 O NPs-decorated TiO 2 nanosheets is rationally designed, and highly selective photocatalytic photoreduction of CO 2 into CH 4 is achieved. The Pd/Cu 2 O/TiO 2 photocatalyst shows a high CH 4 production rate of 42.8 μmol g −1 h −1 with an extremely high selectivity of 99.5%. This CH 4 production rate is 61.1, 5.4, and 2.8 times higher than the bare TiO 2 , Cu 2 O/TiO 2 , and Pd/TiO 2 , respectively. In this Pd/Cu 2 O/TiO 2 hybrid, a consecutive multistep charge transfer is steered between the Cu 2 O/TiO 2 heterojunction and Pd, ensures accelerated charge separation and transfer, and leads to the formation of a spatially separated electron-enriched surface (Pd) and hole-enriched surface (Cu 2 O). This spatially oriented charge transfer and the charge-enriched catalyst surface synergistically contribute to the simultaneous high conversion rate and selectivity of CH 4 .
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Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 2
·777-792
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IF 2.081
Liu Yingxin,Zhang Kaiyue,Zhang Liang,Wang Yun,Wei Zuojun
The selective reductive amination of levulinic acid (LA) into pyrrolidone derivatives is regarded as one of the most promising reactions in the fields of biomass conversion into high value-added chemicals. Herein, we report a one-pot synthesis of N -substituted-5-methyl-2-pyrrolidones by reductive amination of LA/ester with nitriles over several commercial catalysts. Among the catalysts texted, Pd/C was found to be the most efficient for the reductive amination of LA/ester with various nitriles to give high yields of pyrrolidones (up to 92%) under mild reaction conditions (80 °C, 1.6 MPa H 2 , tetrahydrofuran solvent). And the catalyst showed good reusability.
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Green Energy & Environment
·
2021
·
IF 8.207
Jiaqin He,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu
Improving catalytic performance is a yet still challenge in thermal catalytic oxidation. Herein, uniform mesoporous MnO 2 nanosphere-supported bimetallic Pt–Pd nanoparticles were successfully fabricated via a SiO 2 template strategy for the total catalytic degradation of volatile organic compounds at low temperature. The introduction of mesopores into the MnO 2 support induces a large specific surface area and pore size, thus providing numerous accessible active sites and enhanced diffusion properties. Moreover, the addition of a secondary noble metal can adjust the O ads /O latt molar ratios, resulting in high catalytic activity. Among them, the catalyst having a Pt/Pd molar ratio of 7:3 exhibits optimized catalytic activity at a weight hourly space velocity of 36,000 mL g −1 h −1 , reaching 100% toluene oxidation at 175 °C with a lower activation energy (57.0 kJ mol −1 ) than the corresponding monometallic Pt or non-Pt-based catalysts (93.8 kJ mol −1 and 214.2 kJ mol −1 ). Our findings demonstrate that the uniform mesoporous MnO 2 nanosphere-supported bimetallic Pt–Pd nanoparticles catalyst is an effective candidate for application in elimination of toluene.
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JOURNAL OF CONTROLLED RELEASE
·
2021
·
IF 9.776
Minglu Zhou,Chaohui Luo,Zhou Zhou,Lian Li,Yuan Huang
Triple negative breast cancer (TNBC) with highly metastatic features generally does not respond to anti–programmed cell death 1 ligand 1 (PD-L1) therapy due to multiple immunosuppressive mechanisms to exclude and disable T cells . Here, we develop a polymer-based combinatory approach consisting of both immunogenic cell death (ICD)-inducing and CXCR4-inhibiting function to prime tumor microenvironment and improve anti-PD-L1 therapy in TNBC. Our findings revealed that the combination therapy was able to spur the T cell response in primary tumors by increasing the tumor immunogenicity to recruit T cells, removing the physiological barriers of intratumoral fibrosis and collagen to increase T cell infiltration , and reducing the immunosuppressive cells to revive T cells. Meanwhile, such approach efficiently inhibited the formation of pre-metastatic niche in abscopal lung. Because of the significant promotion of anti-tumor and anti-metastasis immunity, the non-responding TNBC gained robust responsiveness to anti-PD-L1 therapy which resulted in complete eradication of orthotopic tumors, inhibition of pulmonary metastasis , and durable memory effects against tumor recurrence . Our work provided a generalizable approach of simultaneous ICD induction and CXCR4 blockade to apply anti-PD-L1 therapy in TNBC.
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Nanomaterials
·
2020
·Vol. 10
·期 8
·1612
·
IF 4.324
Zhaoyu Wen,Qiong Fu,Jie Wu,Guangyin Fan
Simple and efficient synthesis of a nano-catalyst with an excellent catalytic property for hydrogen generation from hydrolysis of dimethyl amine-borane (DMAB) is a missing piece. Herein, effective and recycled palladium (Pd) nanoparticles (NPs) supported on soft nitriding porous carbon (NPC) are fabricated and applied for DMAB hydrolysis. It is discovered that the soft nitriding via a low-temperature urea-pretreatment induces abundant nitrogen-containing species on the NPC support, thus promoting the affinity of the Pd precursor and hindering the agglomeration of formed Pd NPs onto the NPC surface during the preparation process. Surface-clean Pd NPs with a diameter of sub-2.0 nm deposited on the NPC support (Pd/NPC) exhibit an outstanding catalytic performance with a turnover frequency (TOF) of 2758 h−1toward DMAB hydrolysis, better than many previous reported Pd-based catalysts. It should be emphasized that the Pd/NPC also possesses a good stability without an obvious decrease in catalytic activity for DMAB hydrolysis in five successive recycling runs. This study provides a facile but efficient way for preparing high-performance Pd catalysts for catalytic hydrogen productions.Keywords:nano-catalyst;dimethyl amine-borane;palladium nanoparticles;hydrolysis;soft nitriding
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SEMICONDUCTOR SCIENCE AND TECHNOLOGY
·
2020
·Vol. 35
·期 9
·095030
·
IF 2.361
Zhiqiang Yao,Xi Wang,Man Yang,He Ma,Yanfeng Sun,Hong Zhang,Tianwei Dong,Weifeng Liu
Doping of noble metals into semiconductors is often used to enhance the response of gas sensors, accompanying the decrease of the particle size. In this work, pure and palladium-doped dispersive nanoscale tin dioxide nanoparticles with abundant surface defects are synthesized efficiently via a facile hydrothermal method. In the experiment, glucose is used as the carbon source to limit the growth of crystals through the carbonization process and create abundant surface defects after high temperature calcination. Compared with pure SnO2, Pd doping only slightly decreases the particle size with the increase of palladium doping amount from 11.9 nm to 9.6 nm. A gas-sensing investigation indicates that the sensor devices based on pure and 1 at%, 3 at%, 5 at% palladium-doped SnO2 show an obvious high response to n-butanol. In particular, the response to n-butanol reaches to the maximum with the palladium doping amount of 3 at%, and the response increases from 33.3 to 92.9 to 100 ppm n-butanol compared with pristine SnO2 nanoparticle at optimal working temperatures. A gas-sensing mechanism related to surface defects, chemical and electrical sensitization is also discussed.
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JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Xiqiang Tian,Muhammad Zahid,Jiang Li,Wang Sun,Xiaoyu Niu,Yujun Zhu
The addition of a suitable co-catalyst is an encouraging way to enhance the catalytic performance of Pd based catalyst with low content. Herein, we describe an easy synthesis of Mo 2 N-TiO 2 with well-dispersed Mo 2 N nanoparticles through one pot evaporation-induced self-assembly and nitridation treatment method. Moreover, a green bio-reductive approach with Catalpa Fruit ( CF ) extract was adopted to fabricate Pd/Mo 2 N-TiO 2 catalysts for promoting selective hydrogenation of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) as model reaction. Among these Pd/Mo 2 N-TiO 2 catalysts, 0.8 wt%Pd/Mo 2 N-TiO 2 exhibits significantly high catalytic activity for selective hydrogenation of various nitrophenols and cinnmaldehyde. Importantly, the catalytic activity of the catalyst prepared by the reduction method of the CF extract is higher than that prepared by the reduction method of NaBH 4 . A serials of characterization, including XRD, N 2 adsorption–desorption, TEM, XPS, CO chemisorption and CO-FTIR etc., was carried out to investigate the influence of the prepared method on the surface Pd species and activity. The high performance can be attributed to the specific nanostructure characteristics of the catalyst and the good synergistic effect between Pd and Mo 2 N, improving the dispersion of Pd nanoparticles atoms and the exposure of more active Pd atoms (surface Pd 0 species) on 0.8 wt%Pd/Mo 2 N-TiO 2 due to the CF extract as reductant.
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