Polymers
·
2022
·Vol. 14
·期 21
·4647
·
IF 4.967
Hao-Kun Cai,Zhong-Yi Jiang,Siyuan Xu,Ying Xu,Ping Lu,Jian Dong
Hydrogen gas production can be produced from dimethylamine borane by the catalytic effect of metal nanoparticles. Past research efforts were heavily focused on dehydrogenation in organic solvents. In this study, hydrolysis of the borane in aqueous solutions was investigated, which bears two significant advantages: that two-thirds of the hydrogen generated originate from water and that the hydrogen storage materials are non-flammable. Polymer hydrogels serve as good carriers for metal particles as catalysts in aqueous solutions. Kinetic analysis of hydrogen production was performed for Ni/Pd bimetallic nanoclusters dispersed in a polymer hydrogel with a 3-D network structure. The reaction catalyzed by the bimetallic nanoclusters has an activation energy of only 34.95 kJ/mol, considerably lower than that by Ni or other metal catalysts reported. A significant synergistic effect was observed in the Ni/Pd bimetallic catalysts (Ni–Pd = 20/1) with a higher activity than Pd or Ni alone. This proves the alloy nature of the nanoparticles in the borane hydrolysis and the activation of water and borane by both metals to break the O–H and B–H bonds. The hydrogel with the Ni/Pd metal can be recycled with a much longer lifetime than all the previously prepared catalysts. The aqueous borane solutions with a polymer hydrogel can become a more sustainable hydrogen supplier for long-term use.Keywords:hydrogen production;hydrolysis;dimethylamine borane;polymer hydrogel;Ni/Pd alloy nanoparticles;mechanism
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiaolan Li,Yangqi Huang,Zhenyu Chen,Shuqi Hu,Jinliang Zhu,Panagiotis Tsiakaras,Pei Kang Shen
A series of tri-functional nanoflower (NF) catalysts with numerous nanodendrites (Pt 3 NiRh, Pt 3 NiRu, Pt 3 NiPd, Pt 3 Ni, and Pt 2 Ni 2 Rh NFs) were synthesized by introducing Rh, Ru, and Pd into Pt-Ni nanoflowers, aiming at accelerating the sluggish kinetics of oxygen reduction reaction (ORR), methanol oxidation reaction (MOR), and hydrogen evolution reaction (HER). The as-prepared catalysts displayed superior anti-poisoning ability and excellent activity due to uniform morphology and good dispersibility. Their electrochemical characterization revealed that the Pt 3 NiRh NFs showed the highest mass activity (2.17 A m g P G M - 1 ) and specific activity (3.13 mA cm -2 ) toward ORR, close to 9.9 and 4.6 times higher than the values measured on Pt/C (46.7 %). As for MOR, mass and specific activities of Pt 3 NiRh NFs were 1.88 A m g P G M - 1 and 2.62 mA cm -2 , far exceeding the values on commercial Pt/C. Moreover, HER activity of Pt 3 NiRh NFs outperformed commercial Pt/C. This work is valuable to develop promising multi-functional catalysts with enhanced activity and anti-poisoning ability.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Haichuan Zhang,Zede Yi,Shiyu Fu,Changzhi Li,Lucian A. Lucia,Qiying Liu
A rational design of the intrinsic lattice structure of catalysts is vitally important to address catalytic performance. Herein is reported a top-down synthesis for the fabrication of a bifunctional metallic catalyst. First, palladium nanocubes with (100) lattices planes were synthesized through a shape-control strategy; next, the as-synthesized Pd/Co-ZIF was used as a template for in - situ phase reconstruction by a spontaneous phase transformation process in the presence of H 4 SiW under solvothermal conditions. Ultimately, formation of 3D hierarchical flower-like bimetallic nitride nanosheets (SiW 12 @Pd/Co-ZIF-NS) were generated because of this process. The SiW 12 @Pd/Co-ZIF-NS catalyst not only displays excellent catalytic transfer hydrogenolysis for C-O bond cleavage of lignin dimeric substrates, but also maintains superior recycling durability due to an encapsulation phenomenon preventing aggregation. Finally, the resulting nanocomposites exhibit superior activity and good size selectivity toward catalytic transfer hydrogenolysis of the actual lignin substrates to produce a significant amount of low-molecular-weight aromatic compounds .
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 34
·16043-16049
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IF 3.3
Hongbo Yu,Fei Zhang,Shuibo Wang,Yang Cong,Shiwei Wang,Lin Zhu
Hydrodeoxygenation of lignin-derived phenolic compounds to produce alkanes is a promising method used for mitigating fossil energy consumption, but they often require high temperature and high pressure, resulting in their poor catalytic stability and durability. In this study, we encapsulated ∼3.9 nm active metal Rh nanoparticles (NPs) into ∼40 nm hollow mesoporous aluminosilicate nanospheres (HMANs) to synthesize M@Alx–mSiO2 nanoreactors with adjustable Al contents for guaiacol hydrodeoxygenation. The optimized Rh@Al2.0–mSiO2 catalyst displayed significantly enhanced guaiacol activity and cyclohexane selectivity relative to the Rh@mSiO2 catalyst under mild reaction conditions. According to the characterization results, the high hydrodeoxygenation activity of Rh@Al2.0–mSiO2 could be attributable to the synergistic effect between the metallic Rh and Lewis and Brønsted acid sites, and the introduction of Al species greatly facilitated the adsorption of 2-methylcyclohexanol, thereby enhancing cyclohexane selectivity. The confinement effect of Rh NPs inside the hollow cavities effectively prevents the leaching and aggregation of Rh NPs, thereby improving their catalytic durability and stability.
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JOURNAL OF CATALYSIS
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2023
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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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APPLIED SURFACE SCIENCE
·
2023
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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
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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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JOURNAL OF CATALYSIS
·
2023
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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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
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2023
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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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CRYSTENGCOMM
·
2023
·Vol. 25
·期 14
·2110-2118
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IF 3.1
Shi-Jun Yin,Li-Xian Li,Feng-Qing Yang
A polyhedral MIL-125-NH2@Pd nanoparticle with light-responsive oxidase-like activity was synthesized through a simple solvothermal method and was characterized by field emission scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray powder diffraction, Fourier transform infrared spectroscopy, thermogravimetric analysis, Brunauer–Emmett–Teller analysis, etc. MIL-125-NH2@Pd can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) under light radiation without H2O2, indicating its intrinsic light-responsive oxidase-like characteristic. MIL-125-NH2@Pd shows a superior catalytic activity and higher affinity to TMB, compared to MIL-125-NH2, owing to the presence of homogenously distributed palladium (Pd) nanoparticles. The results of the mechanism study indicate the existence of ˙O2− and electron holes during the catalytic reaction of MIL-125-NH2@Pd. Furthermore, based on the excellent light-responsive oxidase-like activity and specific recognition capacity for casein phosphopeptides (CPP) of titanium ions (Ti4+) in MIL-125-NH2@Pd, a simple colorimetric sensing platform was developed for the determination of CPP in a linear range of 10–100 μg mL−1 with a limit of detection as low as 2.9 μg mL−1. Finally, the developed method was successfully employed in the sensitive and selective detection of CPP in spiked rabbit and rat plasma samples. This study may provide a reliable and highly efficient strategy to realize the excitation-responsive sensing applications of materials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Kaiyang Xu,Yu Chen,Hua Yang,Yuyan Gan,Lizhi Wu,Li Tan,Yihu Dai,Yu Tang
Cyclohexanone is an important raw material for manufacturing nylon and other chemicals. The sustainable conversion of biomass derived molecules to cyclohexanone is desired but still challenging. Herein, a palladium single atom catalyst anchored in the micropores of zeolite (namely Pd 1 /ZSM-5) is designed and exhibits remarkable catalytic activity in transforming anisole to cyclohexanone in water medium (H 2 O), without using of organic solvent or halogen promoter. The selectivity to cyclohexanone is 91.2% and the turnover rate (TOR) is 400.8 h −1 at 453 K. The Pd sites, acid sites, and microporous confinement environment of zeolite cooperate to promote the partial hydrogenation to cyclohexanone, and inhibit further hydrogenation as the side reaction. H 2 O not only acts as the solvent, but also participates significantly in the partial hydrogenation. Moreover, as revealed by isotope labelled experiments (D 2 O and H 2 18 O), the water participated hydrogenolysis and the consequent partial hydrogenation mechanism is proposed.
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