CATALYSIS LETTERS
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2022
·Vol. 153
·期 4
·1215-1226
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IF 2.936
Wang Shiqing,Li Yafei,Lan Xiaocheng,Liu Boyang,Wang Tiefeng
Ni phosphide and Lewis acid–base pair site of Al 2 O 3 were combined as highly efficient catalyst for direct amination of 1-octanol to 1-octylamine. Due to the higher dehydrogenation activity and the site isolation effect, Ni 3 P/Al 2 O 3 -TPP prepared by organophosphorus was 4.0 times more active than Ni/Al 2 O 3 and increased the selectivity to 1-octylamine from 71.4 to 92.8% at 0.4 MPa NH 3 . Graphical Abstract
研究领域:
催化化学
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材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Haifan Wang,Menglei Yuan,Jingxian Zhang,Yiling Bai,Ke Zhang,Bin Li,Guangjin Zhang
Ammonia (NH 3 ) synthesis at mild conditions by electrocatalytic nitrogen reduction (eNRR) has received more attention and has been regarded as a promising alternative to the traditional Haber–Bosch process. Lewis acid-base pairs (LPs) can chemisorb and react with nitrogen by electronic interaction, while the tuning of the microenvironment near electrode can hinder hydrogen evolution reaction (HER) thus improving the selectivity of the eNRR. Herein, the FeOOH nanorod coupled with LPs on the surface (i.e., Fe, Fe–O) was synthesized, which could effectively drive eNRR. Meanwhile, polyethylene glycol (PEG) was introduced to serve as a local non-aqueous electrolyte system to inhibit HER . The prepared FeOOH-150 catalyst achieved outstanding eNRR performance with an NH 3 yield rate of 118.07 μg h −1 mg cat −1 and a Faradaic efficiency of 51.4 % at −0.6 V vs. RHE in 0.1 M LiClO 4 + 20 % PEG . Both the experiment and DFT calculations revealed that the interaction of PEG with Lewis base sites could optimize nitrogen adsorption configuration and activation.
研究领域:
化学
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材料科学
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电化学
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DOI
PubMed
高影响因子
Journal of CO2 Utilization
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2021
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IF 7.132
Jiaxin Liang,Shuxian Ye,Wenjing Wang,Congxiao Fan,Shuanjin Wang,Dongmei Han,Wei Liu,Yan Cui,Limin Hao,Min Xiao,Yuezhong Meng
Bulk terpolymerization of carbon dioxide and phthalic anhydride with propylene oxide is successfully carried out using metal-free and economical Lewis pairs under mild conditions. A series of commercial organic bases are coupled with triethyl borane (TEB) as Lewis pairs to optimize the activity and the results show that the TEB/ bis(triphenylphosphine)iminium chloride (PPNCl) pair exhibits relatively high activity and selectivity. The impact of the molar ratio of TEB to organic bases, reaction temperature and CO 2 pressure as well as the catalyst loading on the activity and selectivity of the copolymerization are investigated. Particularly, the turnover frequency reaches 164 h −1 with a TEB/PPNCl molar ratio of 2/1 at 80 °C. To our delight, the poly(ester- co -carbonate)s with random or block structures can be simply tuned by choosing different organic bases coupled with TEB. In these cases, the resultant terpolymers with comprehensive properties can be readily synthesized. As expected, the incorporation of phthalic anhydride effectively modifies the thermal and mechanical properties of commercial poly(propylene carbonate) (PPC). Terpolymers named as PPC-P with 43 mol% aromatic polyester moieties displays a glass transition temperature ( T g ) of 47 °C, about 9 °C higher than that of commercial PPC, and gives a tensile strength higher than 37.6 MPa. To our delight, the synthesized PPC-P exhibits satisfactory degradation speed under standard composting condition compared with commercial PBAT and PPC.
研究领域:
材料科学
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化学工程
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高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2024
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IF 3.8
Sun Baohong,Cui Xin,Zhang Jiachen,Tang Yawen,Sun Hanjun
Hydrolytic nanozyme–based visual colorimetry has emerged as a promising strategy for the detection of aluminum ions. However, most studies focus on simulating the structure of natural enzymes while neglecting to regulate the rate of hydrolysis-related steps, leading to low enzyme-like activity for hydrolytic nanozymes. Herein, we constructed a ruthenium dioxide (RuO 2 ) in situ embedded cerium oxide (CeO 2 ) nanozyme (RuO 2 /CeO 2 ) with a Lewis acid–base pair (Ce–O-Ru-OH), which can simulate the catalytic behavior of phosphatase (PPase) and can be quantitatively quenched by Al 3+ to achieve accurate and sensitive Al 3+ colorimetric sensing detection. The incorporation of Ru into CeO 2 nanorods accelerates the dissociation of H 2 O, followed by subsequent combination of hydroxide species to Lewis acidic Ce–O sites. This synergistic effect facilitates substrate activation and significantly enhances the hydrolysis activity of the nanozyme. The results show that the RuO 2 /CeO 2 nanozyme exhibits a limit of detection as low as 0.5 ng/mL. We also demonstrate their efficacy in detecting Al 3+ in various practical food samples. This study offers novel insights into the advancement of highly sensitive hydrolytic nanozyme engineering for sensing applications.
研究领域:
分析化学
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纳米生物学
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环境科学
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PubMed
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Zhe Hong,Xin Wang,Yingsen Fang,Lihua Deng,Lei Li,Zhirong Zhu
Toluene side-chain alkylation with methanol for the styrene monomer formation remains a great challenge. An optimal synergy between acidic and basic sites on zeolites is required for an efficient catalysis process. It is important to modulate the surface Lewis acid–base pairs precisely. Herein, we report a strategy to restructure the surface Lewis acid–base pairs in cesium-modified X zeolite (CsX) by N doping. In the process of toluene side-chain alkylation, the CsX-BN-600 catalyst, where N species is doped into the framework of the X zeolite, exhibits 2.7 times the styrene formation rate and a much better selectivity of 85.7% in comparison to the parent CsX of 70.1% selectivity to styrene at the same reaction conditions. The introduction of N species into zeolites acts as a new Lewis base site and optimizes the Lewis sites due to its ability of electron donation. Meanwhile, the frustrated Lewis pair (FLP) between the deprotonated framework nitrogen in X zeolite and positively polarized C species in the side-chain alkylation reaction is created. Furthermore, the N doping contributes to the generation of the active intermediates of HCOO* and H3CO*. These reasons favor the superiority of the catalyst through N doping.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Dongjie Zhang,Yue Zhang,Haitao Li,Yin Zhang,Peiru Zhang
Catalytic transfer hydrogenation (CTH) strongly relies on the synergistic interaction between Lewis acid and Lewis base. Highly active, high-density, and well-dispersed Lewis acid–base pairs (LP) are crucial to achieving efficient CTH catalysis, yet forming such an ideal interface remains challenging. To address this, a novel construction strategy is presented, which leverages the regulation of the layered double hydroxide (LDH) lattice structure to establish an ideal LP interface. Supercritical isopropyl alcohol (SCIP) was employed to selectively remove hydroxyl groups and hydrogen bonds from the NiAl-LDH surface, constructing rich MCUS and Ni-OOH at the LDH interface in a simple, controllable, and environmentally friendly way. The formation process of MCUS and Ni-OOH in SCIP was analyzed using a series of dynamic characterization. Key factors restricting the formation of MCUS and Ni-OOH were identified by comparing results across different precursor preparation methods and temperatures of SCIP treatment. On this basis, the one-pot reaction system was established. Within this system, catalyst preparation and the CTH of ethyl levulinate (EL) to γ-valerolactone (GVL) co-occur. The system simplifies the CTH reaction process and exhibits ultrahigh catalytic efficiency, with a GVL formation rate of 0.780 molGVL·g–1·h–1. Compared to traditional reaction systems and catalysts, the developed one-pot reaction system and catalyst demonstrates significant advantages and exhibit excellent cyclic stability after catalyst stabilization. The combination of the LP interface and the one-pot reaction system enabled environmentally friendly, economical, and efficient biomass-based GVL synthesis.
研究领域:
化学
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催化材料科学
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高影响因子
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