Results in Engineering
·
2025
·
IF 7.9
Yuan Zhou,Shaojie Zheng,Hao Lei,Liu Liu,Zhenting Xie,Yanxiao He,Nianbing Zhong,Shuai Xiao,Xuefeng He
The electrochemical CO 2 reduction reaction (eCO 2 RR) provides a sustainable route for producing high value-added syngas through renewable electricity. Nevertheless, the low solubility of CO 2 and the competing hydrogen evolution reaction in eCO 2 RR systems often restrict product selectivity and conversion efficiency. In this study, we propose a microenvironment engineering strategy by incorporating hydrophobic SiO 2 aerogel into Ag nanoparticle (NP) catalysts to enhance reaction kinetics. Experimental results demonstrate that the Ag NPs/20 wt.% SiO 2 -300 electrode delivers a peak CO Faradaic efficiency (FE CO ) of 85.7% at −1.5 V vs. Ag/AgCl in an H-cell, marking a 71.0% improvement compared to the bare Ag NP electrode (50.1%). In-situ Fourier-transform infrared spectroscopy verifies a *COOH-mediated reaction pathway, where the modified catalyst surface promotes intermediate enrichment due to enhanced mass transport. Furthermore, the membrane electrode assembly reactor equipped with the Ag NPs/20 wt.% SiO 2 -300 cathode maintains high FE CO (79.2% to 88.7%) across a broad current range (25 to 150 mA cm −2 ). The CO/H 2 ratio can be precisely adjusted by varying the applied current density, allowing tailored syngas production. This study highlights the pivotal role of hydrophobic microenvironments in modulating product selectivity and presents a scalable method for designing gas diffusion electrodes suitable for industrial eCO 2 RR applications.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Du Wei,Gao Feng,Cui Peng,Yu Zhiwu,Tong Wei,Wang Jihao,Ren Zhuang,Song Chuang,Xu Jiaying,Ma Haifeng,Dang Liyun,Zhang Di,Lu Qingyou,Jiang Jun,Wang Junfeng,Pi Li,Sheng Zhigao,Lu Qingyi
The reversible transformation of a nanohelix is one of the most exquisite and important phenomena in nature. However, nanomaterials usually fail to twist into helical crystals. Considering the irreversibility of the previously studied twisting forces, the reverse process (untwisting) is more difficult to achieve, let alone the retwisting of the untwisted crystalline nanohelices. Herein, we report a new reciprocal effect between molecular geometry and crystal structure which triggers a twisting-untwisting-retwisting cycle for tri-cobalt salicylate hydroxide hexahydrate. The twisting force stems from competition between the condensation reaction and stacking process, different from the previously reported twisting mechanisms. The resulting distinct nanohelices give rise to unusual structure elasticity, as reflected in the reversible change of crystal lattice parameters and the mutual transformation between the nanowires and nanohelices. This study proposes a fresh concept for designing reversible processes and brings a new perspective in crystallography.
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Molecular Catalysis
·
2023
·
IF 4.6
Wenyan Jia,Maoshuai Li,Mingchan Chen,Jing Lv,Mei-Yan Wang,Xiaojun Bao,Xinbin Ma
The epoxide methoxycarbonylation is essential for the synthesis of advanced aldehydes and polyols, but the reaction mechanism has not been well resolved yet. In this work, we have established more detailed mechanism pathways for ethylene oxide methoxycarbonylation over Co-based complexes, the reaction pathway of the main by-product acetaldehyde, and examined the effect of nitrogen-containing heterocycles on the pathways using DFT calculation and experimental study. The conversion of ethylene oxide and product selectivity is sensitive to the structure of nitrogen-containing heterocycles. The addition of pyrazole as a ligand generated the highest conversion (98.3%) and dramatically inhibited by-product (e.g., acetaldehyde, 2-methoxyethanol) formation with the highest selectivity of methyl 3-hydroxypropionate (84.3%). The calculations reveal that the epoxide ring opening is the rate-determining step and the homonuclear ion pair mechanism is the most energetically preferred pathway. The ligand with promoting effect on the methyl 3-hydroxypropionate formation rate can lower the energy barrier of the ring-opening step with a proportional correlation established.
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MOLECULES
·
2022
·Vol. 27
·期 22
·7998
·
IF 4.927
Hui Zhang,Huahui Zeng,Mengfei Li,Yagang Song,Shuo Tian,Jing Xiong,Lan He,Yang Liu,Xiangxiang Wu
A series of co-crystals of ascorbic acid were prepared with equimolar amounts of co-crystal formers (CCFs), including isonicotinic acid, nicotinic acid, 3,4-dihydroxybenzoic acid, 2,5-dihydroxybenzoic acid and m-hydroxybenzoic acid, by slow solvent evaporation and solvent-assisted grinding. The co-crystals were characterized by single-crystal X-ray diffraction spectroscopy, powder X-ray diffraction, IR spectroscopy, differential scanning calorimetry and thermogravimetric analysis. Molecular dynamics (MD) simulations further validated the interaction energy and the possible intermolecular hydrogen bonds among VC and CCFs. The co-crystals showed improved stability when exposed to different wavelengths of light, pH and temperatures compared to the free analogue, especially at higher pH (~9) and lower temperature (~4 °C).Keywords:co-crystals;ascorbic acid;improved stability;hydrogen bonding
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CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 67
·e202201968
·
IF 5.02
Shujue Xu,Shen Zhang,Yang Yu,Shengrui Zhang,Minjie Li
Graphical Au(I)-thiolate nanosheets with closely-packed multiple surface functional groups have been synthesized via a one-pot co-assembly strategy. The easy but powerful strategy addresses the surface engineering problem for 2D materials and paves the way for their wider applications in sensing and biomaterials. Two-dimensional (2D) Au(I)-thiolate assemblies are a special type of material that can balance high structural stability and rich surface functionality, which shows promising prospects in both fundamental research and applications. Co-assembly of multiple ligands is a facile way to further enrich the surface properties and functions, and expand their application potentials. In this work, taking 3-mercaptopropionic acid (MPA), cysteine (Cys) and 1-thioglycerol (TGO) as example ligands, we studied in detail the possibility to co-assemble them into one nanosheet. Although the three ligands have significantly different controllability and pathways when self-assembling individually with Au(I), they can still be effectively co-assembled by reacting with HAuCl 4 together to obtain three-ligand nanosheets with good colloidal stability. The key points for successful co-assembly are also revealed by comparing single- and three-ligand self-assembly processes, laying a solid foundation for co-assembly of even more ligands. The easy but powerful strategy for 2D materials with closely-packed and multiple tunable surface functional groups addresses the surface engineering problem for 2D materials and paves the way for their wider applications in sensing and biomaterials.
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CATALYSIS COMMUNICATIONS
·
2022
·
IF 3.51
Baohuai Zhao,Baofang Jin,Xiaodong Wu,Duan Weng,Rui Ran
A series of Sm-Mn oxides (SmMnO 3 , SmMn 2 O 5 and Sm 0.9 Ag 0.1 Mn 2 O 5 ) of perovskite-type and mullite crystal phases were synthesized for the catalytic oxidation of CO and C 3 H 8 . The Sm 0.9 Ag 0.1 Mn 2 O 5 composition showed the highest catalytic activity among the series of solids, especially for the CO oxidation to CO 2 with T 50 and T 90 values of 60 and 95 °C, respectively. The catalysts were characterized by powder XRD, Raman, BET, XPS, and H 2 -TPR. It was found that the catalytic performance of the solids was correlated well with their redox properties. Synergetic effects between Ag-related species and the mullite phase resulted in more active surface oxygen species and remarkably lowered the reduction temperature of the Sm 0.9 Ag 0.1 Mn 2 O 5 solid.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yongsong Ma,Kaifa Du,Yifan Guo,Mengyi Tang,Huayi Yin,Xuhui Mao,Dihua Wang
Greenhouse gases carbon dioxide (CO 2 ) can be converted into high value-added carbon materials by molten salt electrolysis. Herein, we employ CO 2 as the inorganic carbon source to prepare a core–shell catalyst (Co@C) by molten salt electrolysis for the activation of peroxymonosulfate (PMS) to degrade diethyl phthalate (DEP). The electrolytic Co@C catalyst presents a high catalytic performance for the degradation of DEP with a high turnover frequency (TOF) value (2.28 min −1 ), a relatively low catalyst dosage (Cat = 50 mg L –1 ), low oxidant concentration (PMS = 0.46 mM), a wide range of pH applicability (pH = 3–9), and low activation energy ( E a = 38.88 kJ mol −1 ). In addition, the Co leaching rate is low (<1 mg L –1 ) in the pH range of 5–11 and the total organic carbon (TOC) removal was reached 78.9% under the catalyst dosage was 50 mg L –1 . The DEP degradation pathways mainly involved ethyl formate elimination, ethoxy abstraction, carboxyl abstraction, decarboxylation, hydroxy abstraction, esterification and ring cleavage of DEP. Further, theoretical calculations confirm that Co nanoparticles (Co NPs) encapsulated with graphitized carbon shell derived from CO 2 reduce the work function (WF) of catalysts, enhance the length of bond O–O ( I O-O ) of PMS molecule, and facilitate the charge transfer from the catalysts to PMS molecule. This work provides a new insight into the utilization of CO 2 served as inorganic carbon sources and the design of heterogeneous catalysts.
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MATERIALS LETTERS
·
2021
·
IF 3.423
Lijian Song,Xiahua Zuo,Ying An,Jin Zhan,Youchen Zhang,Weimin Yang,Jing Tan,Lisheng Cheng
Dopamine (DA) has been applied in surface chemistry because of its green and simple polymerization process. However, the polymerization kinetics is slow for mass production. Herein, we proposed a novel method to increase the polymerization rate of DA significantly. The DA solution was treated by a two-step method using microwave irradiation and oxygen oxidation . As a result, the DA solution turned dark only in 6 min. The UV–vis spectra and molecular dynamics showed that microwave irradiation promotes the generation of reactive oxygen species, and the oxygen is used as a supplement to compensate for the overflow of oxygen during the microwave heating process. This study provides a new promising choice to polymerize DA quickly and will inspire related applications in various fields.
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MOLECULES
·
2026
·Vol. 31
·期 18
·3281
·
IF 5.1
Junli Xu,Weilin Zheng,Wanpeng Sun,Zhaoyu Wang
In this study, we report the facile synthesis of perovskite CoTiO3nanorods and their application as an efficient, noble-metal-free cocatalyst for visible-light-driven photocatalytic CO2reduction to CO. Under optimized conditions (MeCN/H2O/TEOA, λ > 420 nm), CoTiO3-600 enhanced the CO yield by more than 15-fold compared to the system without CoTiO3, achieving 29.9 μmol of CO after 1 h of irradiation. Isotopic labeling with13CO2confirmed that the evolved CO originated solely from CO2. Mechanistic investigations revealed that CoTiO3facilitates rapid electron transfer and suppresses charge recombination, as evidenced by photoluminescence quenching. Furthermore, the cocatalyst exhibited excellent stability and reusability, with no significant structural changes observed after multiple reaction cycles. Collectively, this work demonstrates that CoTiO3serves as a cost-effective and robust cocatalyst, holding great promise for sustainable photocatalytic CO2fixation.
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BRAZILIAN JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 1.2
Yang Zelong,Yao Pengfei,Qin Haijian,Xia Qing,Yuan Bo,Zheng Chunzhi,Yang Fengli
CO oxidation has attracted much attention in the field of automotive exhaust treatment and fuel cell industrial process. In this study, NiO loaded on the Ta 2 O 5 was prepared and used to catalyze CO oxidation. And the catalyst NiO/Ta 2 O 5 was characterized by Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS). The catalytic performance was evaluated and the mechanism was analyzed. The catalytic performance has been enhanced greatly by combining NiO with Ta 2 O 5 , the catalyst shows excellent activity in a wide CO concentration from 500 to 10,000 ppm, with CO conversion above 90%. In addition, NiO/Ta 2 O 5 has good stability for CO oxidation with no apparent loss of activity for 8 h. The XPS results show that oxygen defects emerged after reaction. The presence of oxygen defects is responsible for the high catalytic activity. Graphical abstract
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CHEMOSPHERE
·
2023
·
IF 8.8
Xingwen Lu,Jiating Li,Wang Xu,Zenghua Qi,Fei Wang
During the struvite recovery process, Cd, a hazardous metal commonly found in waste streams, can be sequestered by struvite. This study investigated the influence of Cd 2+ on the precipitation of struvite. Quantitative X-ray diffraction (QXRD) results showed that the purity of struvite decreased from 99.1% to 73.6% as Cd concentration increased from 1 to 500 μM. Scanning electron microscopy (SEM) revealed a roughened surface of struvite, and X-ray photoelectron spectroscopy (XPS) analysis indicated that the peak area ratio of Cd–OH increased from 19.4% to 51.3%, while the area ratio of Cd-PO 4 decreased from 86.6% to 48.7% as Cd concentrations increased from 10 to 500 μM. The findings suggested that Cd 2+ disrupted the crystal growth of struvite, and mainly combined with –OH and -PO 4 to form amorphous Cd-bearing compounds co-precipitated with struvite. Additionally, Mg-containing amorphous phases were formed by incorporating Mg 2+ with –OH and -PO 4 during struvite formation.
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JOURNAL OF POLYMER SCIENCE
·
2021
·Vol. 59
·期 14
·1528-1539
·
IF 0
Yao Chen,Wenchuan Wang,Dong Xie,Lili Wu,Chaocan Zhang
TPPAlCl-PPN + Cl − binary catalyst (where TPPAlCl is 5,10,15,20-tetraphenylporphyrin aluminum chloride, PPN + Cl − is bis[triphenylphosphine] iminium chloride, the molar ratio of TPPAlCl to PPN + Cl − is 1 to 0.5) can initiate the effective one-pot/one-step ternary copolymerization of CO 2 , lactide and 4-vinyl-1-cyclohexene-1,2-epoxide, and the quaternary copolymerization of CO 2 , propylene oxide, lactide, 4-vinyl-1-cyclohexene-1,2-epoxide, to form multiblock poly(carbonate-co-lactide) products with pendant vinyl group. The ternary copolymerization product composes of polylactide (PLA) block and poy(vinylcyclohexylene carbonate) (PVCHC) block, and the quaternary copolymerization product composes of poy(propylene carbonate) (PPC) block, PLA block and PVCHC block, which are verified by 1 H NMR, 13 C NMR, 1 H- 1 H cosy, hetero-nuclear multiple bond correlation, DTG, and Gel permeation chromatography analysis. The functionality and glass-transition temperature of the products can be easily adjusted by the copolymerization variables, such as the molar ratio of comonomers, copolymerization temperature, pressure of CO 2 , the concentration of the catalyst. Graphical
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