JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Xiao-Chao Chen,Guang-Hui Shi,Tian-Hong Jing,Yi-Ying Zhuang,Xiao-Li Zhao,Yong Lu,Ye Liu
The acid-base adducts ( A and B ) as the ionic salts in the format of [ L- 2H] 2+ [OTf] 2 − , derived from the neutralization of t -butyl-substituted diphosphines [ L1 : 1,2-bis[(di- tert -butylphosphanyl)methyl]benzene; L2 : 4,5-bis(di- tert -butylphosphino)-9,9-dimethylxanthene] with triflic acid (HOTf, CF 3 SO 3 H), were synthesized, characterized, and then applied in Pd-catalyzed methoxycarbonylation-aminolysis tandem reaction for the synthesis of linear primary amides. For the first time, the structural configurations of such adducts were deconvoluted by the single crystal X-ray diffraction analysis. In A , the two P-H bonds were distinct, and one of the P-H bond was hydrogen-bonded with CF 3 SO 3 − -anion whereas the two P-H bonds in B were equivalent without hydrogen-bond effect. A became more robust against moisture and oxygen than its counterpart of L1 due to the available hydrogen-bond interaction whereas B became more labile in comparison to L2 . When A was applied in Pd-catalyzed methoxycarbonylation-aminolysis tandem reaction, the linear primary amides were obtained in the yields of 69–84% whereas B led to the poor result. It was found that A- Pd(OAc) 2 system not only successfully catalyzed the first-step methoxycarbonylation of alkenes to generate the carboxylic esters with L/B > 90/10 by predominantly following anti -Markovnikov’s rule, but also accelerated the second-step aminolysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Junjing Li,Menghua Yin,Yu Wang,Liang Wang
In order to change the mass transfer efficiency of conventional flat plate electrodes in the catalytic process, a new filtered Pd@Ti electrode has been prepared. The results indicated that the filtered Pd@Ti electrode had the best removal efficiency of 99.59% on diclofenac (DCF) at the flux of 40.85 L/m 2 ∙h -1 . Compared to unfiltered Pd@Ti electrodes, the removal efficiency was 1.18 times higher, the current efficiency was 2.15 times higher and the cost of electricity was 69.05% lower. The electrocatalytic hydrodechlorination process of DCF by filtered Pd@Ti electrode mainly relies on indirect reductive dechlorination by H* adsorbed on the electrode surface. The removal efficiency of the filtered Pd@Ti electrode remained above 80% after six cycles. The removal mechanism and reaction pathway of filtered Pd@Ti electrode for dechlorination of different chlorinated PPCPs were proposed. Furthermore, the ecotoxicity of chlorinated PPCPs and their products were evaluated by using the toxicity estimation software tool (T.E.S.T.) model. This study confirmed the promising application of filtered Pd@Ti electrodes for the removal and detoxification of chlorinated PPCPs in wastewater.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Ruhui Hu,Suyun Zhong,Hezhen Liu,Yawen Liu,Hongxia Chen,Xiaojun Hu
A dual-ligand Cu-MOFs (Cu-F/Hs) based on phenylalanine (Phe) and histidine (His) was innovatively constructed with enhanced catalytic property. Among them, Phe can interact with the dopamine (DA) to enhance the substrate affinity. Meanwhile, the coordination of His with copper ions was inspired by the active site structure of natural laccase to improve the catalytic activity. The K m value of Cu-F/Hs was 0.14 times of laccase, indicating a high affinity for the catalytic substrate DA. Accordingly, a sensitive sensor for PD-L1 detection was designed by using Cu-F/Hs, which can catalyze DA to form redox-active polymeric conjugates deposited on the electrode surface with good electrical conductivity, thereby contributing a “signal-down” electrochemical response with a double signal enhancement. The detection limit was 0.12 ng/mL in the detection range of 0.5 – 200 ng/mL. This work provided a new and simple way to synthesize MOFs with high substrate affinity and efficient activity, and a general signal amplification strategy induced by the catalytic deposition.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Lei Wang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Jie Ding,Li Zhu,Jing Ma,Wenxin Ji,Liqiong Wang,Yuanyuan Li
Dual activation of molecular and lattice oxygen is an important step in the catalytic oxidation of volatile organic compounds. Herein, CeO 2 was derived from MOF as an electron donor support to develop a co-catalyst with Pt-Pd alloy nanoparticles (Pt-Pd/CeO 2 ). The Prepared Pt-Pd/CeO 2 exhibits excellent catalytic activity towards toluene oxidation, showing a turnover frequency (TOF 0.26 s −1 ) higher than those of Pt/CeO 2 (0.05 s −1 ) and Pd/CeO 2 (0.02 s −1 ). Several in situ experimental techniques and density functional theory calculations have revealed that the introduction of Pd valence electrons can intensify the electronic metal-support interactions (EMSIs) effects of Pt-Pd/CeO 2 catalysts, which can weaken the Ce-O bond, thereby promoting the production and circulation of lattice oxygen and oxygen vacancies, and modulating the d -band centre to enhance the adsorption and activation of reactants. This study presents a comprehensive investigation of toluene oxidation on alloy-supported catalysts, providing practical guidance for designing reliable catalysts suitable for industrial applications.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Huijie Wang,Qi Liu,Mengyang Xu,Chenlong Yan,Xianghai Song,Xin Liu,Huiqin Wang,Weiqiang Zhou,Pengwei Huo
The localized surface plasmon resonance (LSPR) effect has shown significant progress in enhancing the efficiency of light absorption and separating photogenerated carriers. Herein, the dual-plasma enhanced 2D/2D/2D g-C 3 N 4 /Pd/MoO 3-x (CPM) S-scheme heterojunction photocatalysts were synthesized using the method of hydrothermal and electrostatic self-assembly for high-selectivity photocatalytic reduction of CO 2 to produce CO. The dual LSPR effect of MoO 3-x and ultrathin Pd nanosheets synergistically broadened the optical response range of the CPM composites and successfully improved the photocatalytic activity and near-infrared (NIR) performance. The optimized CPM-30 photocatalysts exhibited CO yields of 18.55 μmol g −1 with a selectivity of 96.3%. In addition, the CO yield reached 3.92 μmol g −1 after 4 h of NIR light photoirradiation. The electron spin resonance (ESR) and ultraviolet photoelectron spectroscopy (UPS) tests showed that the S-scheme heterojunctions were constructed by coupling g-C 3 N 4 /Pd nanosheets and MoO 3-x . This work will provide a reference for improving product selectivity through the design of two-dimensional composites and the utilization of plasma materials.
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FUEL PROCESSING TECHNOLOGY
·
2023
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IF 7.5
Jia Wang,Jianchun Jiang,Dongxian Li,Xianzhi Meng,Arthur J. Ragauskas
This study focuses on developing advanced oxygen-containing biofuels with high furan, cyclic ketone, and ethanol content from holocellulose and cellulosic wastes. To achieve this, we employed an integrated process that combined hydropyrolysis and vapor-phase hydrodeoxygenation using Pd/Al 2 O 3 as a catalyst. In the first stage, the non-catalytic hydropyrolysis of hemicellulose resulted in furfural and acetic acid fractions that were effectively converted into furans, cyclic ketones, and ethanol in the second-stage reactor over Pd/Al 2 O 3 under 0.3 MPa H 2 . We found that a hydropyrolysis temperature of 440 °C in the first stage reactor resulted in the highest yield of oxygen-containing biofuels (171.1 mg/g) with 89.2% hemicellulose conversion. However, increasing the hydrodeoxygenation temperature in the second stage reactor reduced the yield of oxygen-containing biofuels, and at 400 °C, excess deoxygenation led to hydrocarbon production. The Pd/Al 2 O 3 catalyst demonstrated high stability during the vapor-phase hydrodeoxygenation of primary furfural and acetic acid intermediates, with only 2.1% coke formation after three reaction cycles. This scalable process enables the conversion of various cellulosic wastes into advanced oxygen-containing biofuels, with considerable total yields. Our findings suggest that this integrated process holds great promise for converting biomass waste into advanced oxygen-containing biofuels.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Yuan Shu,Xiaolan Duan,Qiang Niu,Rongyong Xie,Pengfei Zhang,Yunxiang Pan,Zifeng Ma
Zinc oxide is a key material in catalysis. Designing of ZnO crystal aggregates with the surface defect has received significant attention. Herein, we synthesized ZnO aggregates with tiny primary nanoparticles through a mechanochemistry-assisted salt-templating (potassium chloride) method. Interestingly, this KCl-templating strategy could lead to significant increase in specific surface area (SSA) of ZnO (up to 91 m 2 /g), whereas commercial ZnO-COM has a SSA of 5 m 2 /g. Meanwhile, this strategy via ZnCl 2 -KCl solid solution has also created a number of oxygen vacancies into ZnO aggregates. With these attractive features, as-made Pd-ZnO catalyst showed outstanding performance in methanol steam reforming, especially at low temperature (20 % Conversion and 95 % CO 2 Selectivity at 150 °C). Current strategy provides a gateway for the rational design of ZnO-based catalytic materials.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 41
·10666-10676
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IF 5.236
Peng Zhang,Shaonan Xu,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Peiping Zhang,Shiding Miao
Graphical One man‘s trash is another man‘s treasure : A novel template strategy allows fibrous struvite—a composite Pd/Mg 2 P 2 O 7 with a mesoporous structure and an ultrahigh surface area—to be synthesized from wastewater. The prepared Pd/Mg 2 P 2 O 7 nanowires showed excellent performance in the selective hydrogenation of nitrobenzenes. This strategy provided a new pathway for synthesizing highly efficient catalysts as well as a solution for alleviate eutrophic pollution caused by N- and P-containing substances in wastewater. A highly efficient heterogeneous catalyst Pd/Mg 2 P 2 O 7 was fabricated by combining palladium nanoparticles (PdNPs) and mesoporous Mg 2 P 2 O 7 fibers/rods. Mg 2 P 2 O 7 fibers with ultra-high specific surface area were prepared from struvite as templates, which were synthesized from waste water containing N- and P-containing pollutants. This strategy provided a novel pathway for developing advanced catalysts from eutrophication-polluted water. The composite Pd/Mg 2 P 2 O 7 showed brilliant performance in selective hydrogenation of nitro aromatics to give anilines. As an example of nitrobenzene hydrogenation, the conversion to aniline and selectivity were found to reach almost 100 % at a temperature of T =90 °C and under a pressure of P =2.0 MPa. The superior performance was found to originate from PdNPs, which were boosted by electron transfer afforded by the nanofiber Mg 2 P 2 O 7 supports. The favorable adsorption of withdrawing groups (−NO 2 ) was realized by synergistic effects between Pd and oxygen vacancies provided by pyrolysis of struvite. The catalyst remained stable after cycles of reuse with little degradation in catalytic performance.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Jiayu Song,Shengping Wang,Yan Xu,Qingling Liu,Yujun Zhao
Poor catalytic activity and stability are primary defects of traditional Pd/Al 2 O 3 catalysts for the low-temperature methane combustion. Herein, we developed a facile way to synthesize a MgAl-LDHs derived MgAl 2 O 4 spinel with good crystalline lattice and high surface area, which was used as support of Pd-based catalysts. Catalysts with Mg/Al ratio of 1/3 presented the highest methane combustion activity. It was found the well-crystallized MgAl 2 O 4 spinel promoted the dispersion and crystallization of PdO due to the strong interaction between PdO and support, and the electrophilicity and basicity originated from Mg doping suppressed the sintering of PdO particles, leading to the excellent performance of Pd/MgAl3. Moreover, these factors also inhibited the formation of surface OH- species, therefore, improved the water resistance. Such a synthesis strategy of the Pd/Mg x Al y derived from LDHs and the roles of MgAl 2 O 4 spinel could pose some meaningful directions for developing high-efficient Pd-based catalysts for the low-temperature methane combustion.
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CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Dongyue Zhao,Yuexi Yang,Zhongnan Gao,Mengxin Yin,Ye Tian,Jing Zhang,Zheng Jiang,Xiaobo Yu,Xingang Li
Herein, we report the excellent De-NO x performance of La 0.7 Sr 0.3 MnO 3 (LSM) perovskite-supported Pd catalysts (Pd-LSM) in alternating lean-burn/fuel-rich atmospheres using C 3 H 6 as reductant and describe the in situ activation of the Pd catalysts via metal-support interaction (MSI) tuning. The NO x reduction conversion of the Pd-LSM catalyst increased significantly from 56.1% to 90.1% and the production of N 2 O was suppressed. Our results demonstrated that this behavior was mainly attributed to the in situ transformation of Pd 2+ into Pd 0 during the reaction. The generated Pd 0 species could readily activate the C 3 H 6 reductant and achieve an eight-fold higher turnover frequency than Pd 2+ for the reduction of NO x . Moreover, excessive MSIs inhibited the in situ generation of Pd 0 , and thereby, lowered the De-NO x activity of the catalyst even at high Pd dispersion. In addition, the Pd-LSM catalysts exhibited much higher S tolerance than conventional Al 2 O 3 -supported catalysts. Our study provides a new approach for analyzing and designing highly active metal catalysts operated under dynamic alternating oxidizing/reducing atmospheric conditions.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Hao Liu,Ya-nan Qin,Hao-yu Li,Li-xue Gai,Qing-da An,Shang-ru Zhai,Zuo-yi Xiao,Li Cui
Noble metal-based catalytic material with maximum utilization is of prime attraction for conserving rare metal resources. Herein, highly dispersion Ni nanoparticles (NPs)-modified N-doped mesoporous carbon material (Ni-N@C) was fabricated by pyrolysis of Ni 2+ /Histidine cross-linked alginate hydrogels. In a step forward, the obtained Ni-N@C nanocatalyst was treated by the solution of Pd 2+ , and tiny amount of Pd NPs were deposited on the surface of Ni via the reducibility of Ni to achieve the high dispersion of precious metals material. In the degradation of highly-concentration p-nitrophenol, the catalyst presents excellent performance which could completely degrade pollutants within a very short period. It was demonstrated that pre-embedded Ni NPs could not only increase the efficiency of Pd NPs but also endow the facile separation characteristic to the catalyst. Besides, the catalyst maintained favorable catalytic capacity even after five reaction cycles. In brief, this work may provide novel guidance for the maximum utilization of noble metal-modified mesoporous N-doped carbon-supported catalysts in practical applications of industrial and the treatment highly-concentration p-nitrophenol.
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BIOMATERIALS
·
2020
·
IF 10.317
Changrong Wang,Xiaoguang Shi,Huijuan Song,Chuangnian Zhang,Xiaoli Wang,Pingsheng Huang,Anjie Dong,Yumin Zhang,Deling Kong,Weiwei Wang
Immunotherapy has revolutionized cancer treatment; however, only a limited portion of patients show responses to currently available immunotherapy regimens. Here, we demonstrate that RNA interference (RNAi) combined with immunogenic chemotherapy can elicit potent antitumor immunity against melanoma. Specially, we developed cationic polymer-lipid hybrid nanovesicles (P/LNVs) as a new delivery system for doxorubicin and small interfering RNA (siRNA) with extensive cytotoxicity and gene silencing efficiency towards B16 cells. The deployment of doxorubicin-loaded P/LNVs augmented the expression and presentation of endogenous tumor antigens directly in situ by inducing the immunogenic cell death of B16 cells through poly(ADP-ribose) polymerase 1-dependent (PARP1) apoptosis pathway; thereby, eliciting remarkable antitumor immune responses in mice. Leveraging dying B16 cells as a vaccination strategy in combination with RNAi-based programmed cell death ligand 1 (PD-L1) knockdown showed efficacy in both prophylactic and metastasis melanoma settings. Strikingly, PD-L1 blockade synergized with a sub-therapeutic dose of doxorubicin triggered robust therapeutic antitumor T-cell responses and eradicated pre-established tumors in 30% of mice bearing B16 melanoma. Our findings indicated that this combination treatment provided a new powerful immunotherapy modality, characterized by markedly increased infiltration of effector CD8 + T cells and effective alleviation of the immunosuppressive microenvironment in tumors. P/LNVs is a versatile and highly scalable carrier that can enable a broad combination of nanomedicine and RNAi, providing new therapeutic strategies for advanced cancers.
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