Journal of CO2 Utilization
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2023
·
IF 7.7
Shibo Yuan,Peng Bai,Yi He,Jiafa Chen,Yicheng Zhao,Yongdan Li
Photocatalytic N-formylation of amines with CO 2 is a promising strategy to convert CO 2 into value-added chemicals sustainably. In this work, a black TiO 2 -supported Cu photocatalyst is prepared through a solvothermal method for the N-formylation of N-methylaniline with NaBH 4 as the reducing agent. Cu nanoparticles and oxygen vacancies are formed on the surface of the photocatalyst after reduction with H 2 , which decreases the band-gap energy and promotes the separation of photogenerated electrons and holes, thereby improving the photocatalytic activity remarkably. A 100 % conversion is achieved after 9 h radiation, and the yield of N -methylformanilide reaches 81 %. Both the amount of NaBH 4 and the pressure of CO 2 show important influences on the activity and selectivity of the photocatalytic process, and the carbon and hydrogen in the aldehyde group are from CO 2 and NaBH 4 , respectively. The photocatalyst also shows promising cycling durability.
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CELLULOSE
·
2018
·Vol. 25
·期 3
·1705-1714
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IF 3.809
Liu Ting,Ding Enyong,Xue Feng
Polymer grafting is an efficient way to obtain functional cellulose nanocrystals. In this work, we used a “macro-RAFT (macromolecular reversible addition–fragmentation chain transfer) agent-assisted” strategy, which adds extra amount of amphiphilic macro-RAFT agent with low molecular weight to graft poly(N,N-dimethylacrylamide) (PDMA) from cellulose nanocrystals. Successful grafting was evidenced by different characterization methods, and a high weight ratio of grafted PDMA was obtained (77.6%). The grafting process was studied through the weight ratio of grafted PDMA, monomer conversion, and the molecular weight of free and grafted PDMA at different reaction time. As a result, we have suggested that there were three types of grafted polymer chains on cellulose nanocrystals in this reaction system and discussed their evolution during the grafting reaction. Finally, we summarized several key factors for successful grafting in this macro-RAFT agent-assisted strategy.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 33
·11530-11538
·
IF 4.099
Xuelei Pang,Li Li,Yi Wei,Xudong Yu,Yajuan Li
Two novel luminescent organic–inorganic hybrid materials, Ln(L-SBA15)3phen (Ln = Eu, Tb), were designed and synthesized. The organic ligand phenylurea was modified by the silane coupling agent 3-(triethoxysilyl)propyl isocyanate (TESPIC) to form a precursor (L), which was covalently bonded onto a mesoporous SBA-15 backbone to form mesoporous L-SBA15 through co-hydrolysis and co-condensation reactions. 1,10-Phenanthroline monohydrate (phen) was selected as the second ligand to improve the luminescence of the final products, and the two mesoporous hybrid materials Ln(L-SBA15)3phen were obtained after the coordination reaction between the organic ligands (phen and L-SBA15) and Ln(III) ions. Both the mesoporous hybrid materials were examined by Fourier transform infrared spectroscopy, transmission electron microscopy, small-angle X-ray diffraction, N2 adsorption–desorption curves, and photoluminescence spectroscopy. The results show that both the hybrid materials showed highly ordered mesoporous structures, high surface areas, and excellent photophysical properties (long luminescence lifetimes and high quantum efficiencies). Furthermore, the fluorescence sensing properties of the materials were investigated systematically, and the hybrid materials were revealed to be promising examples of dual functional materials with good ability to sense fluoride ions and a small organic molecule N,N-dimethylformamide.
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JOURNAL OF LUMINESCENCE
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2018
·
IF 2.732
Xuelei Pang,Tao Yu,Fengjuan Shen,Xudong Yu,Yajuan Li
Two novel luminescent lanthanide acylamide derivatives covalently grafted to xerogels (donated as Ln-pp-xerogel, Ln = Eu, Tb) were designed and synthesized in situ via a sol-gel process. The properties of these xerogels were examined by Fourier-transform infrared spectroscopy, scanning electron microscopy, X-ray diffraction, thermo-gravimetric analysis, and photoluminescence spectroscopy. The results suggest that the lanthanide derivatives were successfully covalently bonded to the inorganic silica host. The obtained xerogel materials exhibit good thermal stabilities and possess the excellent characteristic luminescence of the corresponding lanthanide ions, which is ascribed to the energy transfer from the organic ligands to the lanthanide ions via an antenna effect. Both the xerogels in acetonitrile solution were used to selective recognition of F − ions and small organic molecule N, N-dimethylformamide by measuring the change in the signal output, which were studied by fluorescence spectroscopy in detail. The sensing mechanisms were studied by the titration of 1 H NMR spectroscopy.
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JOURNAL OF MOLECULAR LIQUIDS
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2016
·
IF 2.74
Caili Dai,Zhe Yang,Yifei Liu,Mingwei Gao,Guochao Zheng,Sisi Fang,Wenjun Wu,Mingwei Zhao
The surface adsorption and micelle formation of N -alkyl- N -methylmorpholinium bromide ([Mor 1,n ]Br n = 12, 14, 16) in aqueous solution is investigated in this work. Through surface tension measurements, the effectiveness of surface tension reduction (∏ cmc ), the maximum surface excess concentration (Γ max ) and the minimum area (A min ) occupied per surfactant molecule at the air/water interface at 25 °C can be deduced. Moreover, the critical micelle concentration (cmc) and various thermodynamic parameters (the standard Gibbs energy (ΔG m 0 ), the enthalpy (∆ H m 0 ), and the entropy (∆ S m 0 )) are calculated by the electrical conductivity measurements at different temperatures. The results of thermodynamic parameters show that the micellization process is driven by entropy.
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ACS Biomaterials Science & Engineering
·
2016
·
IF 0
Wei Wei,Xiaoliang Qi,Junjian Li,Gancheng Zuo,Wei Sheng,Jianfa Zhang,Wei Dong
Poly(N,N-diethylacrylamide) is not only a thermosensitive polymer, but also a good hydrogen bond acceptor. Therefore, drugs with carboxyl groups can serve as hydrogen bond donors and form interactions with the tertiary amide groups in N,N-diethylacrylamide. Herein, we report a novel drug delivery system for anionic drugs composed of poly(N,N-diethylacrylamide) and salecan. Salecan was used to improve the hydrophilicity and accelerate the responsive rate of this system. As expected, salecan-enriched hydrogels exhibited higher swelling ratios and were more sensitive to temperature. Moreover, scanning electron microscopy images showed that the hydrogels are superporous structures, with pore-sizes that increase with salecan concentration. The swelling ratios decreased continuously with the increase of temperature in the range 25–37 °C. MTT assay for cell viability and cell adhesion studies confirm the cell compatibility of the system. Delivery tests using diclofenac sodium, an anti-inflammatory drug, indicate that the thermosensitive property of this system is favorable for anionic drug delivery. Interestingly, the release rates of diclofenac sodium from the hydrogels were temperature dependent, with higher temperatures contributing toward faster release rate.
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REACTIVE & FUNCTIONAL POLYMERS
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2014
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IF 2.822
Suo-Hong Zhi,Ran Deng,Jun Xu,Ling-Shu Wan,Zhi-Kang Xu
Polyacrylonitrile (PAN)-based composite membranes were prepared by immersion precipitation method by using poly( N , N -dimethylaminoethyl methacrylate)-grafted silica (PDMAEMA@SiO 2 ) nanoparticles as hydrophilic additives. The molecular weight of PDMAEMA were controlled by the surface initiated atom transfer radical polymerization of N , N -dimethylaminoethyl methacrylate on SiO 2 nanoparticles. The synthesized nanoparticles have a typical core–shell structure as characterized in detail by FT-IR, TEM , DLS and GPC . The prepared PAN-based composite membranes have higher porosity and water permeation flux than those of the pure PAN membranes. They also show high rejection (⩾90%) to bovine serum albumin and high flux recovery ratio (⩾90%) to water permeation. These improved performances are attributed to the good hydrophilicity of PDMAEMA@SiO 2 nanoparticles. The results suggest that PDMAEMA@SiO 2 nanoparticles are suitable for the property optimization of PAN-based composite membranes.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2017
·
IF 3.671
Ting Liu,Enyong Ding,Feng Xue
Natural polymer flocculants for wastewater treatment have received close attention in recent years. Here we used two flocculants, polyacrylamide and poly( N , N -dimethylacrylamide) grafted cellulose nanocrystals synthesized by a “macro-RAFT assisted” strategy, for the flocculation of kaolin suspension. The flocculation performance of these two flocculants, including flocculants dosage, settling time and floc size, was carefully studied and compared. Results suggested that poly( N , N -dimethylacrylamide) grafted cellulose nanocrstyals showed better flocculation performance than polyacrylamide grafted ones. Meanwhile, their flocculation behavior was also compared with other cellulose-based flocculants in literature and we suggested polymer modified cellulose nanocrstals as flocculants might have higher flocculation performance, but this needs further verification.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yatao Yang,Xiaoxiao Ding,Zequan Zeng,Weihong Jiao,Yifan Li,Yaqin Hou,Zhanggen Huang
TiO 2 -based catalysts are extensively employed in flue gas pollution control processes, including volatile organic compounds (VOCs) oxidation and selective catalytic reduction (SCR). Nonetheless, there persists challenges related to the lack of a clear mechanistic understanding and high N 2 selectivity for the selective oxidation of nitrogen-containing volatile organic compounds (NVOCs). Herein, titania nanotube-supporting transition metals oxides catalysts were prepared to degrade N, N-dimethylformamide (DMF). The results manifested that the interaction between metal and support (M−O−Ti) could enhance oxygen vacancy (O v ), hence promote the DMF decomposition. CuTi catalyst with high O v content exhibited the highest activity and N 2 selectivity for DMF decomposition. In situ diffuse reflectance infrared fourier transform spectroscopy (DRIFTs) and density functional theory (DFT) calculation also proved that CuTi catalyst facilitated the degradation of DMF into dimethylamine (DMA). Moreover, the MnTi catalyst with higher content of lattice oxygen was advantageous in facilitating the complete degradation of DMF into CO 2 , which enhanced CO 2 selectivity. This study could provide theoretical guidance for the practical industrial degradation of NVOCs using TiO 2 -based catalysts.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Jia Shunhan,Zhang Libing,Liu Hanle,Wang Ruhan,Jin Xiangyuan,Wu Limin,Song Xinning,Tan Xingxing,Ma Xiaodong,Feng Jiaqi,Zhu Qinggong,Kang Xinchen,Qian Qingli,Sun Xiaofu,Han Buxing
Nitrogen oxides (NO x ) play important roles in the nitrogen cycle system and serve as renewable nitrogen sources for the synthesis of value-added chemicals driven by clean electricity. However, it is challenging to achieve selective conversion of NO x to multi-nitrogen products (e.g., N 2 H 4 ) via precise construction of a single N-N bond. Herein, we propose a strategy for NO x -to-N 2 H 4 under ambient conditions, involving electrochemical NO x upgrading to NH 3 , followed by ketone-mediated NH 3 to N 2 H 4 . It can achieve an impressive overall NO x -to-N 2 H 4 selectivity of 88.7%. We elucidate mechanistic insights into the ketone-mediated N-N coupling process. Diphenyl ketone (DPK) emerges as an optimal mediator, facilitating controlled N-N coupling, owing to its steric and conjugation effects. The acetonitrile solvent stabilizes and activates key imine intermediates through hydrogen bonding. Experimental results reveal that Ph 2 CN* intermediates formed on WO 3 catalysts acted as pivotal monomers to drive controlled N-N coupling with high selectivity, facilitated by lattice-oxygen-mediated dehydrogenation. Additionally, both WO 3 catalysts and DPK mediators exhibit favorable reusability, offering promise for green N 2 H 4 synthesis.
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Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 48
·41813-41823
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IF 9.5
Ying Meng,Rui Yin,Yanqi Wu,Jie Biao,Guohuang Kang,Feiyu Kang,Yidan Cao
The severe interfacial reaction between the lithium metal anode and the ester-based electrolyte hinders the application of lithium metal batteries. While lithium nitrate (LiNO3) can stabilize the electrode–electrolyte interface, its poor solubility in ester-based electrolytes limits its effectiveness. To address this, we develop a polymerized N,N-dimethylacrylamide (PDMAA)-mediated organic–inorganic composite artificial solid electrolyte interphase (SEI) formed via thermal polymerization of a precursor containing N,N-dimethylacrylamide (DMAA) and LiNO3. DMAA not only exhibits a high donor capacity, facilitating high-concentration LiNO3 dissolution, but also strongly coordinates with H2O molecules, effectively reducing the generation of aggressive hydrofluoric acid (HF) in the electrolyte. The abundant LiNO3 effectively contributes to stable, ion-conductive interphases on both the cathode and the anode. The artificial SEI, through synergistic organic–inorganic interactions, enables uniform lithium deposition, stabilizes the cathode structure, and suppresses the electrolyte hydrolysis. As a result, the symmetric cell achieves stable cycling for over 600 h with a low overpotential (∼34 mV), and the full cell maintains 81.6% capacity after 500 cycles. The cell also exhibits excellent rate-performance attributed to the enhanced interfacial kinetics and moisture-resistance capability due to the scavenging effect of water by PDMAA. This artificial SEI design strategy extends the applicability of LiNO3 in ester-based electrolytes for high-performance lithium metal batteries.
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AICHE JOURNAL
·
2025
·
IF 4
Qi Liu,Yan Ouyang,Tong Luo,Qinlan Luo,Min Xiao,Hongxia Gao,Zhiwu Liang
Blending is a common method to improve the performance of amine solution for CO 2 capture. While the amine will degrade at elevated temperatures or so-called thermal degradation, the mixing of multiple amines could change the thermal degradation behavior and it is critical to reveal them before implementing the CO 2 capture at large scale. Herein, the thermal degradation performance of blended amines was studied via experimental and computational methods. In comparison with single amine solution, the effect of an additional tertiary amine N,N -dimethylethanolamine (DMEA) was analyzed. The thermal degradation experiments were carried out at multiple temperatures. The temperature threshold was identified for the blended solution after which the degradation rate increases dramatically. Based on the obtained degradation products, the degradation mechanism of the blended amine is proposed. The energy barrier of key reactions in thermal degradation was obtained and the interaction of primary amine and tertiary amine is clarified.
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