CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Maonan Ran,Guan Zhang
The NO 3 − electroreduction process presents a promising alternative to the Haber-Bosch method by offering dual benefits: removal of nitrates from wastewater coupled with efficient NH 3 production. Herein, Mo and S doped Fe 3 O 4 nanoplates grown on foam Fe (Mo-S-Fe 3 O 4 @FF) with electron-rich Mo δ+ state was synthesized through a facile hydrothermal approach. Notably, Mo-S-Fe 3 O 4 @FF electrode achieved a nearly fourfold enhancement in ammonium yield compared to foam Fe electrode, while also enhancing the NH 3 Faradaic efficiency. At − 1.3 V vs . Ag/AgCl in a K 2 SO 4 + KNO 3 solution, the Mo-S-Fe 3 O 4 @FF electrode attained a NH 3 Faradaic efficiency of 91.3 %. Furthermore, performance was observed to improve with increasing solution pH levels as the reaction proceeded. From both kinetic and thermodynamic perspectives, our findings demonstrate that high NH 3 production activity is characteristic of Mo-S-Fe 3 O 4 @FF—indicating significant enhancements in conversion rates from NO 3 − →NO 2 − →NH 3 . Theoretical calculation, in conjunction with experimental analyses, reveal that the co-modification of Fe 3 O 4 with Mo and S enhances electron transfer capacity during NO 3 − RR. This modification forms Lewis-acid (Fe-Mo) pairs that increase nitrate adsorption energy alongside Lewis-base (S-O) sites that attract protons, thereby improving overall NO 3 − RR activity. This report elucidates the synergistic effects of Lewis-acid and Lewis-base sites on optimizing catalytic performance for NO 3 − RR using foam Fe-based electrodes.
研究领域:
环境科学
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电催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·
IF 3.5
Peiyao Liu,Zhengzeng Yang,Mengyuan Zhang,Yufeng Liu,Dandan Han,Dan Wu,Charles Chunbao Xu,Jianshe Wang
C-H carboxylation of furoic acid (FA) with CO2 is an atom-efficient strategy to produce 2,5-furandicarboxylic acid (2,5-FDCA) from lignocellulose. The existing carbonate-promoted CO2 carboxylation processes rely on the use of large amounts of expensive Cs2CO3 as deprotonating reagent and molten salt. Substitution of Cs with other cheap and abundant alkali ions (such as K and Na) can reduce the use of Cs, but faces the problem of low yield of 2,5-FDCA. This study found that the addition of catalytic amounts of ZnCl2 as a Lewis acid can increase the yield of 2,5-FDCA in the CO2 carboxylation reaction of Na/K-FA in a molten salt reaction system. 1H NMR analysis and DFT calculations confirmed that ZnCl2 coordinates with the furan ring through electron transfer from the conjugated furan ring to Zn2+, thereby activating the H at the C5 position of Na/K-FA. This coordination lengthened the C5-H bond and lowered its heterolytic dissociation energy, making it more susceptible to being deprotonated by CO32- and subsequently carboxylated by CO2. The developed Lewis acid coordination strategy provides a new idea for the efficient construction of C-C bonds between CO2 and aromatics through carbonate-promoted C-H carboxylation.
研究领域:
化学工程
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可再生资源转化
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催化化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Dongni Liu,Peng Cui,Fangfang Zhang,Hao Ren,Lilin Fang,Xiaosi Sun,Haiyan Ji,Wenshuai Zhu,Zhichang Liu
Ionic liquid is an ideal candidate in the extraction of aromatic compounds. The design and construction of ionic liquids with high extraction efficiency and selectivity towards to the specific aromatics remain crucial question. In this paper, with the aid of orthogonal array experiment, the imidazolium-based ionic liquids with long alkyl chain on the cations were determined to possess high aromatics extraction efficiency. Furthermore, the Lewis acid anion was introduced into the ionic liquid to form 1-dodecyl-3-methylimidazolium ferric chloride ([C 12 mim][FeCl 4 ]) and performed 62 % and 100 % extractant efficiency of naphthalene (NAP) and anthracene (ANT), respectively. Then the porous carbon materials (P1-1000) derived from hyper-crosslinked porous polymers (HCP) which possessed high BET surface area (1186 m 2 /g) was dispersed in [C 12 mim][FeCl 4 ] to form porous ionic liquid. The single extraction efficiency of NAP improved from 62 % to 77 %. The great single extraction efficiency was attributed to the high porosity, additional adsorption sites provided by the Lewis acid anions and the hydrophobic long alkyl chain on the cations. After three times extraction, the concentration of NAP dropped down to 0. The porous ionic liquids also showed good recycle performance. The construction of porous ionic liquids provided an efficient approach for extraction of polycyclic aromatic hydrocarbons from aliphatic hydrocarbon.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Wenfeng Hao,Peng Lu,Xiaosheng Wang,Yuxiang Liu
A simple and facile co-calcination strategy of Beta molecular sieves and cerous nitrate is proposed. Based on the results of XRD , UV–Vis, in-situ FTIR, and 29 Si MAS NMR techniques, open-site configurations of Ce(III)O 4 and Ce(IV)O 4 tetrahedrons are observed due to a large ionic radius of Ce 3+ and Ce 4+ ions. Open-site configurations result in a low ratio of BrØnsted and Lewis acid sites in HBeta-Ce-6. In the isomerization of α- pinene, a higher amount of Lewis acid sites increases the yield for camphene . BrØnsted acids are accessible for α- pinene to form limonene due to a high surface area and low coke deposition. Isomorphous incorporation of Ce 3+ occurs and a decreasing selectivity for limonene are observed using regenerated catalysts. These results indicate that co-calcination strategy protects Beta molecular sieves from thermal destruction, endows Beta molecular sieves with a higher relative crystallinity and porosity during calcination .
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2024
·
IF 4
Mengjiao Yu,Xiong-Fei Zhang,Siting Yang,Yunhua Bai,Zhongguo Wang,Jianfeng Yao
Developing functional catalysts with both Lewis and Brønsted acid sites is an essential task for achieving the direct conversion of glucose to 5-hydroxymethylfurfural (5-HMF), a process that is crucial for the sustainable production of renewable fuels and chemicals. In this work, a mixed-linker strategy is proposed to prepare defective MIL-53(Al)-NH 2 by introducing trifluoroacetic acid into the MIL-53(Al)-NH 2 synthesis process. The creation of defects facilitates the exposure and accessibility of Al 3+ centers, as well as changes the coordination environment within the MIL-53(Al)-NH 2 skeleton. Both the number of Lewis and Brønsted acid sites are boosted, which is beneficial for glucose activation and 5-HMF generation. Through optimizing the reaction conditions, a glucose conversion of 98.3 % with a 5-HMF yield of 59.3 % was achieved by using defective 6d-MIL-53(Al)-NH 2 in a biphasic tetrahydrofuran/H 2 O NaCl system. Moreover, the 6d-MIL-53(Al)-NH 2 catalyst showed excellent recyclability and reusability, with its catalytic efficiency maintained almost unchanged for consecutive 10 cycles. The catalytic mechanism was elucidated and the acidity of the Lewis and Brønsted acid was modulated by defect engineering to achieve exceptional performance.
研究领域:
化学工程
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催化科学
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可再生资源
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jiarun Cheng,Chaojie Lyu,Hongming Chen,Dongsheng Geng,Jinlong Zheng
Elucidating the mechanism of metal-support interface domain regulation is crucial for designing efficient fuel cell electrocatalysts. Herein, we propose an emerging strategy to enhance oxygen reduction reaction (ORR) activity and selectivity by regulating the Lewis alkalinity of carbon support to adjust the Lewis acidity of metal sites. The experimental results and density functional theory (DFT) simulations show that the introduction of N/S atoms into the carbon support structure will break the charge balance of the carbon skeleton and effectively regulate the charge distribution in the Pt-carbon interface domain, thus promoting the oxidation of the Lewis acid Pt atoms to a higher valence state Pt x+ , so as to optimize the adsorption energy of oxygen-containing intermediates. Moreover, Bader charge analysis also verifies that N,S-HMCS, as a Lewis base, can receive more electrons from the Pt sites of Lewis acid, and the electron loss at Pt sites caused by N,S-HMCS strengthens interfacial electron effect. Meanwhile the strong electron adsorption ability of N/S atoms causes the d-band center of Pt atom orbital to shift upward to the Fermi level, which strengthens the binding of metal Lewis acid Pt sites with *OOH intermediates, and improves the 4-electron transfer mechanism. This research reveals the direct role of Lewis acid sites in ORR of fuel cell cathode, and provides a feasible way to guide the design of electrocatalysts with Lewis acid/base double centers.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yuhao Yang,Chunhua Wang,Jiani Cai,Ying-Ya Liu,Zhiquan Yu,Zhichao Sun,Yao Wang,Anjie Wang,Chong Peng
Selective hydrogenation of phenol to cyclohexanone is of great significance for the production of value-added chemical intermediates and products. Pd/MIL-100(Cr), featuring highly dispersed Pd nanoparticles (∼2.5 nm), were synthesized using a double-solvent impregnation method followed by NaBH4 reduction. During aqueous-phase phenol hydrogenation, the catalyst achieved full conversion with 98.3% selectivity toward cyclohexanone within 1 h at 0.1 MPa and 100 °C. The catalyst exhibited high stability, maintaining performance up to 5 cycles without deactivation. The Lewis acidity of MIL-100(Cr) significantly influenced the phenol hydrogenation selectivity. By incorporation of Al, V, and Ce species into the MIL-100(Cr) framework, cyclohexanone selectivity in phenol hydrogenation was found to increase with the amount of Lewis acid sites (LAS). The acid properties of the Pd/MIL-100 catalysts were investigated using NH3-TPD, pyridine-adsorbed FT-IR, and EPR probe molecules. The interaction between Pd nanoparticles and the coordinatively unsaturated sites from the trimeric clusters of MIL-100 was found to be crucial in determining the Lewis acidity of the Pd/MIL-100 catalysts. Demonstrating a synergistic effect between the Pd and LAS, Pd/MIL-100(Cr) emerges as a promising candidate for the selective hydrogenation of phenol to cyclohexanone.
研究领域:
催化化学
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材料科学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Jiarong Qiu,Yi Liu,Jingwen Zhang,Ben Zhou,Qiyue Yang,Liangqing Zhang,Jianfeng Chen,Bingshu Wang,Lu Lin,Xianhai Zeng
A series of zirconium phosphate (ZrP) loaded H-beta-25 zeolite (i.e., ZrP@HB) multifunctional composite catalysts were synthesized by a simple co-precipitation method, and the one-pot upgrading for the transfer hydrogenation of furfural to γ-valerolactone (GVL) was systematically investigated through various characterizations and catalytic evaluation experiments. Comparative characterization analysis of the ZrP@HB-X(Y) catalysts showed that the ZrP@HB-4(4) catalyst has uniform distribution of elements, exhibiting a large specific surface area and hierarchical mesoporous/microporous structure. Fourier transform infrared spectroscopy of pyridine (Py-FTIR) and NH 3 temperature-programmed desorption characterizations indicated the presence of Lewis and Brønsted acid sites, as well as weak, moderate, and strong acid sites in the ZrP@HB-4(4) catalyst. It was confirmed by X-ray photoelectron spectroscopy and FTIR that the main reason for Lewis and Brønsted acid sites formation is the presence of P-O-Zr, P-O-H, and HB zeolite on the ZrP@HB-4(4) catalyst. The HB zeolite as well as Zr and P ratio, can be easily adjusted to efficiently regulate the acidity strength and Lewis and Brønsted acid sites of the ZrP@HB-X(Y) catalysts. The catalytic experiments demonstrated that the physicochemical properties of the ZrP@HB-4(4) catalyst mentioned above significantly enhance the GVL production. Notably, Lewis and Brønsted acid sites as well as transition metal sites of Zr in the ZrP@HB-4(4) catalyst were identified as the main factors that enhance the yield of the target product. By optimizing the reaction conditions, the yield of GVL could be as high as 88.16%. Reusability experiments demonstrate that the ZrP@HB-4(4) catalyst possesses excellent stability. Using levulinic acid as the substrate, the yield of GVL reached 93.92%, suggesting its potential versatility.
研究领域:
催化化学
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可再生化学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 5
·1989-1998
·
IF 3.5
Yanshu Liu,Guanyun Zhang,Dexin Wang,Guanjie Chen,Fangfang Gao,Chen-Ho Tung,Yifeng Wang
A cryptand-like Ti-coordination compound, namely Ti12Cs, comprising two Ti6-salicylate cages and hosting two Cs+ ions, was synthesized by the solvothermal method. It exhibits strong visible-light absorption with an absorption band edge of 652 nm, attributed to the electron transition from salicylate ligands to Ti ions. Electrochemical impedance, visible-light transient photocurrent response, and photoluminescence spectra confirm that Ti12Cs has excellent visible-light response and charge-separation properties. Ti12Cs can be used as a heterogeneous and recyclable photocatalyst for CO2/epoxide cycloaddition, with high utilization efficiency of visible-light under mild conditions. The mechanism investigation points to a synergistic effect of photocatalysis and Lewis acid catalysis.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2014
·
IF 5.825
Qian Wu,Dapeng Wu,Yafeng Guan
Modified nucleosides are important biomarkers of cancers. For their analysis, boronate adsorbents were widely used to selectively capture them from urine, but often suffered from serious secondary hydrophobic interaction and harsh alkaline extraction condition. In this work, the hybrid titania–zirconia nanoparticles coated on porous silica spheres (TiO2–ZrO2/SiO2) were developed for the first time as a selective adsorbent for nucleosides under neutral conditions based on specific recognition of its Lewis acid sites to the cis-diol group. It was found here that TiO2–ZrO2 has higher binding constants than pure TiO2 or ZrO2, and a significant improvement of binding efficiencies was obtained by decreasing calcination temperature to 400 °C. Moreover, physiological pH of urine (pH 6–7) was found optimal to adsorb nucleosides and resist other Lewis base interferences. By self-assembly of TiO2–ZrO2 nanoparticles on silica, unprecedentedly high binding capacity (35 mg/g) for nucleosides was obtained due to high surface area (350 m2/g) and abundant Lewis acid sites on the surface. Due to efficient reduction of secondary hydrophobic interaction on the inorganic surface, cis-diol nucleosides could be captured from 500-fold non-cis-diol interferences. In the real sample application, nine nucleosides have been quantified with relative recoveries in 83%–126%, and 42 ribosylated metabolites had been identified with only 100 μL of urine at physiological pH. Among them, two nucleosides have never been identified in most previous studies using boronate adsorbents for capture.
研究领域:
分析化学
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生物医学工程
·
癌症研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2014
·
IF 5.039
Binbin Jin,Peigao Duan,Yuping Xu,Bing Wang,Feng Wang,Lei Zhang
The activities of several Lewis acid catalysts such SnCl 2 , FeCl 3 , ZnCl 2 , AlCl 3 , and NbCl 5 for the in situ transesterification/esterification of lipid contained within a microalga ( Chlorella pyrenoidosa ) in ethanol at 350 °C were examined to identify the most suitable catalyst in term of crude biodiesel (CBD) yield. Of those catalysts tested, ZnCl 2 showed the highest performance toward the CBD production. Using ZnCl 2 as catalyst, effects of reaction temperature (200–370 °C), time (0–120 min), ethanol to microalga ratio (EtOH:MA) (5/5–40/5), catalyst loading (0–30 wt.%), and algae moisture (0–80 wt.%) on the yields of product fractions and the properties of CBD were studied. The presence of ZnCl 2 not only promoted the production of CBD but also showed activities toward the deoxygenation and denitrogenation of CBD. The moisture content in the starting material is the most influential factor affecting the yield and properties of CBD.
研究领域:
生物化学
·
可再生能源
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Qingrun Meng,Jiaxu Liu,Guang Xiong,Xinyao Li,Liping Liu,Hongchen Guo
The Sn-Beta zeolite is an efficient Lewis acid catalyst for a wide range of chemical reactions. Here a seed-free aerosol-assisted hydrothermal strategy is used to synthesize plate-like Sn-Beta zeolite with higher tin content. A majority of Sn species were transformed into the framework of Beta zeolite as the desired tetrahedral coordination state, which creates strong Lewis acid sites. Moreover, the diffusion property of the Sn-Beta zeolite can be further improved by a mild base-surfactant (NH 3 ˙ H 2 O-CTAB) treatment. The addition of CTAB can not only narrow the mesopore distribution but also prevent the excessive loss of Sn species. The obtained hierarchical Sn-Beta zeolite exhibits an enhanced catalytic performance in the Baeyer–Villiger oxidation of bulky ketone.
研究领域:
催化材料
·
化学工程
·
纳米材料合成
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）