CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ding-Ming Xue,Yi-Jun Zhang,Jing-Wen Chen,Hao Yang,Rui-Jie Xie,Shi-Chao Qi,Yuan-Qing Bu,Fei Liu,Hou-Hu Zhang,Jacques Lalevée
Covalent organic frameworks (COFs), as a newly emerging kind of porous and crystalline materials, serve as an ideal template for hydrogen peroxide (H 2 O 2 ) photosynthesis. However, the vision of achieving high efficiency and selectivity in H 2 O 2 photosynthesis is greatly hindered by the large exciton binding energy and limited charge separation efficiency influenced by the molecular structure of the building blocks. Herein, we developed three newly designed COFs with a donor–acceptor (D-A) structure and incorporated regulatory units (fluorine, F, and methoxyl, OCH 3 ) in the D-A pathway through molecular engineering to optimize electronic structure, the availability of activate sites, charge kinetics and O 2 activation capacity. Due to electron-donating effect, OCH 3 -functionalization (NIES-COF-3) can strengthen the intramolecular electron transfer and interaction with O 2 . This results in a reduction of the energy barrier of the rate-determining step (*O 2 → *OOH) and excellent O 2 -to-H 2 O 2 photocatalytic activity under visible light irradiation, delivering an H 2 O 2 production rate of 3238.4 μmol g −1 h −1 and a high apparent quantum yield of 3.17 %. In addition, F-functionalization (NIES-COF-2) primarily reduces the band-gap energy and improve the O 2 adsorption capacity compared to unfunctionalized NIES-COF-1. This work unveils insight into the catalytic activity-optimization mechanism of molecular engineering in the D-A structure and provides important references for photocatalysts.
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Advanced Science
·
2025
·
IF 14.1
Kun Zhang,Ni Dan,Ruo-Yu Zhang,Jiaojiao Wei,Rui-Xue Tian,Yongfan Zhang,Hong-Ru Fu,Mei Qiu,Lu-Fang Ma,Shuang-Quan Zang
Preparing multi-color and multi-stimuli-responsive circularly polarized luminescence (CPL) materials and understanding the evolution of chirality through the visualized mode is still a challenge. Here, an encapsulation engineering approach of chiral metal-organic frameworks (MOFs) is proposed to confine guest emitters to realize multi-color and multi-stimuli-responsive CPL. Based on triplet-triplet energy transfer (TTET), white CPL and near-infrared circularly polarized room temperature phosphorescence (NIR-CPRTP) can be obtained by introducing the pyrene derivatives. With the introduction of the guest containing vinylpyrene group, the light- and thermal-responsive CPL with the signal inversion can be realized through the reversible [2+2] cycloaddition reaction between the ligand and guest triggered by visible light/ultraviolet light or heating. Furthermore, the excitation-dependent CPL is successfully achieved with the incorporation of excited state intramolecular proton transfer (ESIPT) molecules into nanopores. Importantly, the chirality magnification can be greatly enhanced through the chiral spatial confinement, the accurate host-guest single crystal structures of FLT@DCF-12 and FLT@LCF-12 provide the visualized mode to understand the mechanism of chirality transfer, amplification and responsiveness. White LED and multiple information display and encryption are further demonstrated. This breakthrough provides a new perspective to guest-encapsulated chiral MOFs and contributes to the construction of stimuli-responsive CPL-active materials.
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CHEMICAL ENGINEERING SCIENCE
·
2024
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IF 4.1
Qi Liu,Tong Luo,Yiyan Yin,Yan Ouyang,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Amine degradation is one of the key issues that hampers the implementation of amine-based post combustion carbon capture technology. In this work, the oxidative degradation of fourteen structurally varied amines were experimentally studied by measuring the amine loss, alkalinity change, ammonia yield, and degradation product. There is a linear relationship between amine loss against alkalinity change and ammonia yield, indicating that the degradation product either loss reactivity for CO 2 absorption or emit out as the small molecule. The results have shown that amine stability generally increased with amine order and stronger steric hindrance effect. Most primary and secondary amines showed more than 40 % amine loss after 336 h degradation experiment, while most of tertiary amines showed less than 10 % amine loss. This may be due to the exposed amine groups of primary and secondary amines. The oxidative degradation mechanism was studied based on density functional theory (DFT) calculations.
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PLANT PHYSIOLOGY AND BIOCHEMISTRY
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2024
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IF 6.1
Siyue Liu,Jinge Xie,Wenqi Luan,Chen Liu,Xiwen Chen,Defu Chen
The current trend in agricultural development is the establishment of sustainable agricultural systems. This involves utilizing and implementing eco-friendly biofertilizers and biocontrol agents as alternatives to conventional fertilizers and pesticides. A plant growth-promoting fungal strain, that could alter root system architecture and promote the growth of Arabidopsis seedlings in a non-contact manner by releasing volatile organic compounds (VOCs) was isolated in this study. 26S rDNA sequencing revealed that the strain was a yeast-like fungus, Papiliotrema flavescens . Analysis of plant growth-promoting traits revealed that the fungus could produce indole-3-acetic acid and ammonia and fix nitrogen. Transcriptome analysis in combination with inhibitor experiments revealed that P . flavescens VOCs triggered metabolic alterations, promoted auxin accumulation and distribution in the roots, and coordinated ethylene signaling, thus inhibiting primary root elongation and inducing lateral root formation in Arabidopsis . Additionally, transcriptome analysis and fungal infection experiments confirmed that pretreatment with P . flavescens stimulated the defense response of Arabidopsis to boost its resistance to the pathogenic fungus Botrytis cinerea . Solid-phase microextraction, which was followed by gas chromatography-mass spectrometry analysis, identified three VOCs (acetoin, naphthalene and indole) with significant plant growth-promoting attributes. Their roles were confirmed using further pharmacological experiments and upregulated expression of auxin- and ethylene-related genes. Our study serves as an essential reference for utilizing P . flavescens as a potential biological fertilizer and biocontrol agent.
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JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Kungang Chai,Ke Lu,Zhijun Xu,Zhangfa Tong,Hongbing Ji
A porous crosslinked starch polymer (CSTO) using bitolylene diisocyanate as crosslinker was prepared by a facile method and used to selectively recover acetophenone (AP) from petrochemical effluent mainly containing AP and 1-phenylethanol (PE). The theoretical calculation results indicated that AP exhibited the superior affinity toward the adsorption sites of CSTO through noncovalent interactions. The adsorption measurements showed that, due to the large surface area and high affinity of phenyl rings, CSTO displayed an extremely rapid adsorption rate, a desirable adsorption capacity and selectivity to AP. The adsorption kinetics and isotherms in single solute system agreed well with the pseudo-second-order kinetic model and Freundlich isotherm model, and the adsorption was exothermic and spontaneous. Furthermore, CSTO showed excellent reusability for selective adsorption of AP from equimolar mixture of AP/PE, prompting us to further examine its applicability. In the practical application, CSTO also revealed a fast, preferential and reusable adsorption of AP from actual petrochemical effluent.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Fei Li,Yong Wang,Jian Du,Yong Zhu,Congying Xu,Licheng Sun
Water oxidation as a multi-electron transfer and endothermal reaction has been considered to be the bottleneck of solar-driven water splitting into oxygen and hydrogen. Herein, an alternative approach for solar energy conversion is developed by coupling H 2 generation with the selective oxidation of alcohol. In a closed redox system containing molecular ruthenium catalyst (RuCat) and Pt modified g-C 3 N 4 (Pt-g-C 3 N 4 ) composite, hydrogen production is concomitant with the oxidation of benzyl alcohols to aldehydes with over 99% selectivity in the presence of visible light and pure water. By contrary, the system lacking molecular catalyst only exhibits low to moderate selectivities towards aldehydes. The remarkably improved selectivity is attributed to the formation of highly active Ru(IV) = O intermediate through efficient hole transfer from g-C 3 N 4 to RuCat.
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Royal Society Open Science
·
2018
·Vol. 5
·期 1
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IF 2.504
Guofu Ma,Fengting Hua,Kanjun Sun,Enke Fenga,Hui Peng,Zhiguo Zhang,Ziqiang Lei
The electrochemical performance of an energy conversion and storage device like the supercapacitor mainly depends on the microstructure and morphology of the electrodes. In this paper, to improve the capacitance performance of the supercapacitor, the all-pseudocapacitive electrodes of lamella-like Bi18SeO29/BiSe as the negative electrode and flower-like Co0.85Se nanosheets as the positive electrode are synthesized by using a facile low-temperature one-step hydrothermal method. The microstructures and morphology of the electrode materials are carefully characterized, and the capacitance performances are also tested. The Bi18SeO29/BiSe and Co0.85Se have high specific capacitance (471.3 F g–1 and 255 F g–1 at 0.5 A g–1), high conductivity, outstanding cycling stability, as well as good rate capability. The assembled asymmetric supercapacitor completely based on the pseudocapacitive electrodes exhibits outstanding cycling stability (about 93% capacitance retention after 5000 cycles). Moreover, the devices exhibit high energy density of 24.2 Wh kg–1 at a power density of 871.2 W kg–1 in the voltage window of 0–1.6 V with 2 M KOH solution.
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MACROMOLECULES
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2018
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IF 5.914
Heng Li,Huitong Luo,Junpeng Zhao,Guangzhao Zhang
Alcohol-initiated ring-opening alternating copolymerization (ROAP) of phthalic anhydride (PA) and a variety of mono-, di-, and trisubstituted epoxides has been performed with a weak phosphazene base (t-BuP1) as the catalyst. Each product exhibits a perfectly alternating sequence distribution, controlled molar mass (Mn up to 124 kg mol–1), and low dispersity (ĐM < 1.15, mostly). Full conversion of PA can be reached in 0.5–24 h depending on the substituent of the epoxide, the targeted degree of polymerization, and the amount of t-BuP1 used (0.2–5 mol % of PA) when the reactions are conducted under solvent-free conditions at 100 °C with a small excess of the epoxide (0.5 equiv of PA). The glass transition temperature of the polyester ranges from −14 to 135 °C. The living nature of the ROAP allows one-pot construction of well-defined block-alternating copolymers through sequential addition of two epoxides. Statistical-alternating copolymers have also been synthesized by copolymerization of PA and two mixed epoxides. Thus, the structural diversity of aromatic alternating polyesters synthesized by this simple organocatalysis has been largely enriched.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Pengbo Li,Yuanrong Zhang,Haodi Liu,Yanfen Fang,Shuaitao Li,Xun Hu,Qifeng Chen
The conjugated structure of graphitic polymeric carbon nitrides (GPCNs) has low efficiency in the photocatalytic hydrogen peroxide (H 2 O 2 ) production, due to the electronic properties, band structure, and surface-active-sites. Herein, boron and carbon-ring modified GPCNs were synthesized with via a thermal condensation method, using melamine and phenylboronic acid as raw materials. The introduced boron atom, conjugated to the carbon atom in the heptazine moiety, and the adjacent nitrogen vacancy (V N ) formed a dual-site, which not only modified the electronic properties but also promoted the adsorption and activation of molecular dioxygen; The carbon-ring introduced altered the band structure and electron distribution, which was proved by density functional theory (DFT) calculations. The co-modification promoted the conversion of dioxygen molecule to H 2 O 2 , coupled with oxidation of benzyl alcohol (BA) to benzaldehyde (BAD). The optimal activity was achieved over CN-B 3 (1.87 mmol/(g·h)), which was about 4-fold higher than that of PCN (0.49 mmol/(g·h)). More interestingly, mechanism study revealed that the photocatalytic H 2 O 2 generation was realized via a photon energy transfer route, that is, O 2 molecule firstly was converted to a highly active singlet oxygen ( 1 O 2 ) intermediate, which was reduced by electrons to superoxide anions ( O 2 − ) and coupled with proton to form H 2 O 2 . This method provides a novel strategy to improve photocatalytic H 2 O 2 and high value-added chemical production by regulating the microstructure and electronic structure of GPCNs through heteroatom and moiety co-modification.
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FOOD RESEARCH INTERNATIONAL
·
2024
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IF 7
Jieyao Yu,Jingzhe Li,Zhi Lin,Yin Zhu,Zhihui Feng,Dejiang Ni,Shengchun Zeng,Xuehong Zeng,Yijun Wang,Jingming Ning,Liang Zhang,Xiaochun Wan,Xiaoting Zhai
As a kind of green tea with unique multiple baking processes, the flavor code of Lu’an Guapian (LAGP) has recently been revealed. To improve and stabilize the quality of LAGP, further insight into the dynamic changes in odorants during the whole processing is required. In this study, 50 odorants were identified in processing tea leaves, 14 of which were selected for absolute quantification to profile the effect of processes. The results showed that spreading is crucial for key aroma generation and accumulation, while these odorants undergo significant changes at the deep baking stage. By adjusting the conditions of the spreading and deep baking, it was found that low-temperature (4 °C) spreading for 6 h and low-temperature with long-time baking (final leaf temperature: 102 °C, 45 min) could improve the overall aroma quality. These results provide a new direction for enhancing the quality of LAGP green tea.
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CHINESE JOURNAL OF POLYMER SCIENCE
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2024
·
IF 4.1
Liu Xin-Yu,Zhu Liang,Jie Su-Yun,Li Bo-Geng
Due to their excellent biocompatibility and biodegradability, aliphatic polyesters are widely used in the biomedical, packaging and agricultural fields, which are usually accessed by the ring-opening polymerization (ROP) of lactones and the catalysts particularly play an important role. Herein a series of quinolinyl-urea catalysts have been synthesized via the reaction between isocyanate and aminoquinoline with an amino group at different substitution positions and characterized. In combination with 7-methyl-1, 5, 7-triazabicyclo[4,4,0]dec-5-ene (MTBD) as a cocatalyst and benzyl alcohol (BnOH) as an initiator, 1-(3,5-bis(trifluoromethyl)phenyl)-3-(quinolin-3-yl)urea ( 3-QU ) was observed to be most active for the ROP of δ -valerolactone ( δ -VL). The polymerization conditions were optimized by varying the type of organic base, catalyst concentration and reaction temperature. By changing the ratio of [M] 0 /[I], linear polyvalerolactones (PVLs) with different molecular weights and narrow molecular weight distribution were prepared. The kinetic and chain extension experiments were carried out to prove the “living”/controllable feature. And the NMR experiments were used to support the proposal of possible mechanism.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2025
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IF 6.2
Wen-Ao Shi,Zhong-Hao Jiang,Ni Bai,Ai-Min Wang,Ai-Rong Mao,Zi-Long Zhao,Lin Lang,Jian Wei,Hai-Yan Liu,Qing-Qing Sun,Yong Gao,Yu-Hong Kang,Yan-Jun Li,Jin-Jun Bai
The separation of condensed aromatic compounds from coal tar residue (CTR), converted into cyclanes via catalytic hydroconversion (CHC) to produce essential blending components for coal-based jet fuel, represents a significant strategy for enhancing CTR's value. A highly efficient bifunctional catalyst was prepared by loading Ni nanoparticles (NNPs, ca . 10 %) on β /MCM-41 composite zeolite ( β / M) and denoted as Ni 10 % @ β / M . CTR was sequentially extracted with acetone/carbon disulfide, petroleum ether, and petroleum ether/methanol (5 vol% H 2 O) to obtain the soluble portion in methanol phase (PEEP M ). PEEP M mainly consists of phenols (64.8 %) and arenes (18.9 %). It was conducted to CHC over Ni 10 % @ β / M at 160 °C for 16 h under 5 MPa of an initial hydrogen pressure (IHP) to obtain CHPEEP M . The results indicate that the relative content of cyclanes in CHPEEP M reaches as high as 93.4 %. In Ni 10 % @ β / M , abundant defects, hierarchical porous composite zeolite with strong Lewis acid sites and uniformly dispersed NNPs play crucial roles in removing heteroatoms and hydrogenating aromatic rings (ARs), respectively. Benzyloxybenzene (BOB) is a model compound with a >C-O- bridge bond and ARs, used to study the catalytic activity of Ni 10 % @ β / M . BOB was completely converted into cyclanes at 160 °C for 2 h under 5 MPa IHP. The high yield of polycyclic alkanes is related to the coupling between the active fragments formed after >C-O- cleavage and the main structure. The synergistic transfer of H···H, δ+ H···H δ- , and H + generated by Ni 10 % @ β / M activation of H 2 is key to the hydrogenation of ARs via induced >C-O- bond cleavage, leading to the formation of saturated cyclanes.
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