FUEL
·
2023
·
IF 7.4
Zhongchun Yuan,Tingting Cao,Min Deng,Jun Ma,Shuo Geng,Chunliang Yang,Yuan Ren,Mengqin Yao,Fei Liu,Xiaodan Wang
It is very crucial but still a huge challenge to develop efficient and durable catalysts to promote hydrogen production from formic acid (FA). Herein, three CeO 2 with structurally well-defined different shapes, i.e., sCeO 2 (spheres), rCeO 2 (rod) and oCeO 2 (octahedral), are prepared, and their effect on the crystal faces and oxygen vacancy over the constructed heterostructure catalysts (Pd-CeO 2 /C) have been intensively investigated in the FA dehydrogenation. Pd-sCeO 2 /C outperforms the other catalysts with a turnover frequency (TOF) value of 2691 h −1 and selectivity to hydrogen of 100 % at 30 °C. A synergism between the CeO 2 (1 1 0) facet and more oxygen vacancies is considered to be key to obtaining the high reactivity. Moreover, biomass carbon promotes the dispersion of Pd-CeO 2 heterostructures due to its large specific surface area and causes more defects in the Pd-CeO 2 /C. Combined with in-situ FTIR and density functional theory (DFT), it is speculated that FA is decomposed through formate pathway over the Pd-sCeO 2 /C. This work thus provides a reasonable design and controllable synthesis strategy for the effective application of FA as an available liquid phase hydrogen storage material.
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INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Zexiao Zhang,Jiahui Wei,Bing Yuan,Fengli Yu,Congxia Xie,Shitao Yu
An aqueous phase Pd nanoparticles (NPs) system reduced and stabilized only by sodium lignosulfonate (SLS) was found to exhibit a favorable catalytic performance in hydrodeoxygenation of vanillin to produce 2-methoxy-4-methylphenol (MMP). Ultraviolet-visible spectroscopy (UV-Vis), transmission electron microscope (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared (FT-IR) characterization were carried out to confirm the formation of NPs, and the influence of various metal salt precursors, temperatures, stirring rates and SLS concentrations on catalyst preparation. It was revealed that the optimized Pd NPs with an average diameter of 14.63 nm had achieved a 99.8 % vanillin conversion and a 98.6 % MMP selectivity under the conditions of 1 mmol vanillin, n (Vanillin) / n (Pd) = 300, 1 MPa H 2 , 70 °C and 2 h. Besides, MMP, the target product, was found an auto-separation property from the aqueous catalyst system due to its less solubility in water. Furthermore, this aqueous Pd NPs catalyst was demonstrated to have stable catalytic activity in the hydrodeoxygenation of vanillin by ten-run tests with favorable conversions of vanillin above 98 %. The selectivity of MMP stayed above 92 % within five runs and still maintained 85.4 % after ten runs. Thus, an environmentally friendly and mild-conditioned hydrodeoxygenation method of vanillin into MMP was developed by using SLS, one of the by-products of the pulp and paper industry.
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Nanoscale
·
2022
·Vol. 15
·期 4
·1554-1560
·
IF 8.307
Ziang Guo,Liye Zhu,Xuan Liu,Ran Zhang,Tiying Zhu,Nan Jiang,Yan Zhao,Yijian Jiang
Improving the activity and stability of electrocatalysts for the hydrogen evolution reaction (HER) plays an essential role in the practical application of electrochemical water splitting under alkaline conditions. Here, trace Pd-doped Ru nanoparticles have been achieved using the pulsed laser ablation in liquid technology, which exhibit efficient HER catalytic performance. It is evidenced that the Pd doping amount is maintained at a trace level and increases nonlinearly with the concentration of the Pd precursor. Molecular dynamics simulations demonstrate that the trace doping of Pd is due to the slow thermal decomposition rate of the Pd precursor. This work improves the mechanistic explanation of the metal doping induced by liquid-phase laser ablation, which may promote the fabrication and application of advanced laser-based nanostructures.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jing Yang,Heng-Quan Chen,Fen Qiao,Xifeng Zhu,Tao Wang,Wei-Ping Pan
Engineering metal-based nanoarchitectures and their atomic-scale arrangement is a promising avenue for enhanced mercury adsorbent activities. Interactions between metal single atoms and substrates result in regulated transitions between distinct reaction processes that boost mercury adsorption activity. Herein, a novel sorbent of porous Co 3 O 4 with Palladium atomic dispersed was successfully prepared by one-step pyrolysis of zeolitic imidazolate framework 67 (ZIF-67) precursors. Via engineering single Pd atoms into ZIF-derived Co 3 O 4 (Pd 1 /Co 3 O 4 -ZIF), the strong metal-support interaction (SMSI) activated the reducibility of Co 3+ in porous Co 3 O 4 to efficiently adsorb and oxidize Hg 0 , enhancing its mercury removal efficiency. Specifically, Pd 1 /Co 3 O 4 -ZIF exhibited superior sorption performance for Hg 0 over a broad range of temperatures (30–350 °C) and high gaseous hourly space velocity (about 555,500 hr −1 ) with the average Hg 0 removal efficiency higher than 98%. The strategy of constructing atomic active sites on the surface of porous metal-oxide to convert adsorbed Hg 0 into HgO is a promising approach to solve the problem that Hg 0 in flue gas is challenging to remove. Density functional theory (DFT) calculation further proved that the existence of a single Pd site on the surface of Co 3 O 4 significantly reduced the energy barrier of Hg 0 to HgO at the atomic level. This work contributed to a thorough comprehension of the structural and adsorption properties of the ZIF-derived Co 3 O 4 sorbent engineering with a single atom and enabled the efficient capture of elemental mercury in flue gas by such ZIF-derived sorbent.
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Advanced Healthcare Materials
·
2023
·Vol. 12
·期 17
·2300110
·
IF 10
Shuaiying Wu,Jianzhong Zhang,Jie Pan,Shuang Bai,Ziying Wang,Yulun Chen,Dazhuang Xu,Yibo An,Chao Liu,Chengchao Chu,Qixuan Dai,Lai Jiang,Zhixiang Lu,Gang Liu
It is an engaging program for tumor treatment that rationalizes the specific microenvironments, activation of suppressed immune system (immune resistance/escape reversion), and synergistic target therapy. Herein, a biomimetic nanoplatform that combines oxidative stress with genetic immunotherapy to strengthen the therapeutic efficacy is developed. Ru-TePt nanorods, small interfering RNA (PD-L1 siRNA), and biomimetic cellular membrane vesicles with the targeting ability to design a multifunctional Ru-TePt@siRNA-MVs system are rationally integrated. Notably, the Fenton-like activity significantly enhances Ru-TePt nanorods sonosensitization, thus provoking stronger oxidative stress to kill cells directly. Meanwhile, immunogenic cell death is triggered to secrete numerous cytokines and activate T cells. The effective catalase characteristics of Ru-TePt enable the in situ oxygen-producing pump to improve tumor oxygen level and coordinately strengthen the therapeutic effect of SDT followed. More importantly, anti-PD-L1-siRNA mediated immune checkpoint silence of the PD-L1 gene creates an environment conducive to activating cytotoxic T lymphocytes, synergistic with boosted reactive oxygen species-triggered antitumor immune response. The experimental results in vitro and in vivo reveal that the Ru-TePt@siRNA-MVs nanosystems can effectively activate the oxidative stress-triggered immune response and inhibit PD-1/PD-L1 axis-mediated immune resistance. Consequently, this orchestrated treatment paradigm provides valuable insights for developing potential oxidative stress and genetic immunotherapy.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 15
·5999-6008
·
IF 9.8
Yuanyuan Zhang,Wanxiang Zhang,Yan Wang,Shuhang Ren,Yucui Hou,Weize Wu
To reduce the emission of NO from fossil fuel combustion and the energy consumption associated with NH3 production, the development of simple and efficient methods to transform NO into high-value-added NH3 is essential. Here, we report the efficient catalytic hydrogenation of NO to NH3 under mild reaction conditions by the synergistic catalysis of functionalized ionic liquids (FILs) and Pd catalysts. In this system, an FIL [TEPA][Im] acted as both an absorbent and a catalyst. The presence of [TEPA][Im] enhanced the catalytic performance by changing the coordination and electronic environment of Pd on the Pd/C catalyst. First, NO was absorbed by [TEPA][Im]; then, the hydrogenation of absorbed NO to NH3 was performed at a low temperature via the synergistic catalyzation of [TEPA][Im] and Pd/C. The effects of various factors on NO hydrogenation to NH3 were also investigated. Remarkably, Pd/C exhibited outstanding properties in the formation of NH3 with a high yield of 67% in the FIL [TEPA][Im] under the conditions of 100 °C and an H2 pressure of 0.5 MPa. [TEPA][Im] could be reused multiple times and the product NH3 could be recovered by flashing.
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Molecular Catalysis
·
2023
·
IF 4.6
Wei Tian,Yonggang Dong,Hong Qin,Ziming Luo,Qian Lin,Zheng Chen,Hongyan Pan,Yongyong Shi,Keliang Wang
The direct synthesis of hydrogen peroxide (DSHP) from hydrogen and oxygen is a green synthesis method with a high atomic economy. However, H 2 O 2 selectivity and productivity remain a key challenge, the O O bonds are easily broken with supported Pd catalysts to produce water. Herein, we report the synthesis of bimetallic catalyst PdSn@Pd@HCS by adapting reversed-phase micellar and galvanic replacement reaction. The novel bimetallic yolk-shell structure catalysts exhibit excellent catalytic performance, the selectivity and productivity of H 2 O 2 reaching 98% and 4899 mmol/g Pd· h − 1 , respectively. Theoretical calculations reveal that the presence of Sn inside the bimetallic alloy can enhance the ligand effect and optimize the electronic structure of the surface Pd atoms, weakening the adsorption ability of O 2 molecules and inhibiting the dissociation of O O bonded species, resulting in the enhancement of H 2 O 2 selectivity and productivity. This work provides the groundwork for bimetallic yolk-shell structure catalysts to achieve the efficient synthesis of H 2 O 2 .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Nan Lu,Bin Liu,Zhengxin Peng,Jing Sui,Xiaofan Zhang,Yuting Ma,Renhong Li,Xiaoqing Yan
Rational design and fabrication of catalysts with excellent efficiency, high selectivity and outstanding stability is of great significance for the practical application of formic acid dehydrogenation into hydrogen gas. Herein, Pd catalysts with a narrow size distribution around 2.2 nm are deposited on the porous chitosan microspheres, which are produced by the polycondensation with Schiff base linkage. The Pd–N bond configuration is formed upon the abundant amino-group on the chitosan backbone with the surface anchoring Pd nanocluster. The surface charge is redistributed to generate high-valence Pd δ+ species due to the ligand-to-metal charge transfer between Pd and N, thus greatly improving the catalytic performance of formic acid dehydrogenation at room temperature and maintaining outstanding stability during 15 consecutive reaction cycles. The present work paves the way to the rational synthesis of Pd-based catalysts with tunable electronic states for practical purposes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Gaojie Li,Kai Du,Xinxin Wang,Xiaochen Wang,Boao Chen,Chuangwen Qiu,Jiaqiang Xu
This study is attempted to improve the hydrogen sensing performance of SnO 2 based sensors by simultaneously employing two strategies of morphology control and noble metal loading. Therefore, SnO 2 ultrathin nanosheets with thickness not exceeding 3.5 nm were successfully synthesized by a hydrothermal method and then different content of Pd nanoparticles were uniformly loaded onto SnO 2 surface by in situ reduction with ascorbic acid . The gas sensing properties demonstrated that the introduction of Pd not only altered the selectivity of the SnO 2 sensor from ethanol to hydrogen, but also significantly improved the gas sensitivity and reduced the working temperature. And the optimal 1.0%Pd/SnO 2 sensor owned the highest sensitivity (75), fastest response-recovery property (21 s/13 s) to 20 ppm of hydrogen at 220 °C, and the actual detection limit is as low as 0.1 ppm. Furthermore, 1.0%Pd/SnO 2 sensor exhibited excellent repeatability, reproducibility and acceptable anti-interference of humidity. The DFT studies suggest that the physisorption of the hydrogen molecules on the surface of SnO 2 , but chemisorption on the surface of Pd/SnO 2 . The improved H 2 sensing performance of Pd/SnO 2 sensor attributes its ultrathin thickness of SnO 2 and catalytic dissociation of Pd to O 2 and H 2 .
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MOLECULES
·
2023
·Vol. 28
·期 12
·4731
·
IF 4.6
Ailing Li,Fuping Dong,Yuzhu Xiong
Nitrogen-rich porous organic polymers were fabricated through a nonreversible ring-opening reaction from polyamines and polyepoxides (PAEs). The epoxide groups reacted with both primary and secondary amines provided by the polyamines at different epoxide/amine ratios with polyethylene glycol as the solvent to form the porous materials. Fourier-transform infrared spectroscopy confirmed the occurrence of ring opening between the polyamines and polyepoxides. The porous structure of the materials was confirmed through N2adsorption–desorption data and scanning electron microscopy images. The polymers were found to possess both crystalline and noncrystalline structures, as evidenced by X-ray diffraction and high-resolution transmission electron microscopy (HR-TEM) results. The HR-TEM images revealed a thin, sheet-like layered structure with ordered orientations, and the lattice fringe spacing measured from these images was consistent with the interlayer of the PAEs. Additionally, the selected area electron diffraction pattern indicated that the PAEs contained a hexagonal crystal structure. The Pd catalyst was fabricated in situ onto the PAEs support by the NaBH₄ reduction of the Au precursor, and the size of the nano-Pd was about 6.9 nm. The high nitrogen content of the polymer backbone combined with Pd noble nanometals resulted in excellent catalytic performance in the reduction of 4-nitrophenol to 4-aminophenol.Keywords:porous organic polymer;amine–epoxy;ring opening;catalyst carrier
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BIOORGANIC CHEMISTRY
·
2022
·
IF 5.307
Wenda Zhu,Yiping Fan,Yanbing Li,Lizhi Peng,Yifang Li,Fengxia Yan,Jiaqiang Zhao,Lei Zhang,Hiroshi Kurihara,Rongrong He,Heru Chen
Eight hybrids of amantadine ( ATD ) with a natural modulator gardenamide A ( GA ) via an alkylene carbonyl bridge or alkylene bridge have been designed and synthesized. Evaluated by electrophysiological assay, compound 5b was confirmed an enhanced NMDAR antagonist compared to ATD with IC 50 value of 10.2 ± 1.2 μM. 5b has been demonstrated to reverse the damages of behavioral performance, the loss of dopaminergic neurons, the reduction of TH positive, and the increase of α-synuclein in both MPTP-treated mice and zebrafish models. In both ethological and ecological experiments, the activity of 5b was confirmed better than ATD or ATD/GA combination, and was almost equal to the positive selegiline. In vivo and in vitro , 5b is shown to reverse the ascend of NR1 and i- NOS levels. This candidate was also demonstrated the activity to down-regulated MPTP-increased Ca 2+ influx in SH-SY5Y cells in a steep and sharp mode. It is displayed that 5b exerts neuroprotective effect partly by activating the PI3K/Akt signaling pathway. Taken all together, our data support that 5b is a more promising agent against PD than ATD .
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JOURNAL OF THE ENERGY INSTITUTE
·
2022
·
IF 6.47
Zuqin Duan,Xue Wang,Qian Lei,Honglin Chen
Catalytic dehydrogenation of formic acid (FA) is one strategy to generate hydrogen from an easily handled chemical and meet the clean-energy demand simultaneously. The Pd/N-doped carbon catalyst is famous for boosting the activity of active metal in FA dehydrogenation. However, the origin of achieving highly catalytic activity remains controversial. Herein, a variety of Pd/N-doped carbon catalysts were systematically prepared by regulating different N doping content and reduction conditions (H 2 and NaBH 4 ) for promoting hydrogen production from FA under ambient conditions without additives. The results showed that N dopants have a great impact on the electronic state and particle size of Pd . Moreover, the electronic state of Pd is also sensitive to the reduction methods. The catalyst with the highest pyridinic-N content presented the best catalytic performance after being reduced in H 2 flow at 260 °C, and its initial TOF value is 2656 h −1 without additives at 50 °C. The electronic levels investigation of the active metal can provide new ideas for the design of highly efficient catalysts for FA dehydrogenation.
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