ChemSusChem
·
2015
·Vol. 8
·期 12
·2066-2072
·
IF 7.657
Yehong Wang,Jian Zhang,Jing Liu,Chaofeng Zhang,Zhixin Zhang,Jie Xu,Shutao Xu,Fangjun Wang,Feng Wang
Graphical CO 2 -mediated reactions: CO 2 -mediated metathesis reactions between amines and DMF to synthesize formamides are described. The N -formylation of amines to formamides is achieved by activating amines, not DMF, via a C N and N H bond metathesis reaction. Using this method, primary, secondary, aromatic, and heterocyclic amines as well as diamines can be obtained with good to excellent formamide yields. Herein, we report CO 2 -mediated metathesis reactions between amines and DMF to synthesize formamides. More than 20 amines, including primary, secondary, aromatic, and heterocyclic amines, diamines, and amino acids, are converted to the corresponding formamides with good-to-excellent conversions and selectivities under mild conditions. This strategy employs CO 2 as a mediator to activate the amine under metal-free conditions. The experimental data and in situ NMR and attenuated total reflectance IR spectroscopy measurements support the formation of the N -carbamic acid as an intermediate through the weak acid–base interaction between CO 2 and the amine. The metathesis reaction is driven by the formation of a stable carbamate, and a reaction mechanism is proposed.
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JOURNAL OF ORGANIC CHEMISTRY
·
2019
·
IF 4.745
Na Li,Jinku Bai,Xiaolin Zheng,Honghua Rao
An iron-catalyzed methylene forming strategy is disclosed through sequential C–H and C–O bond functionalization of methanol with cosolvent water. This protocol provides an easy and novel access to methylene-tethered imidazo[1,2-a]pyridine and 2-aminopyridine analogues in a sustainable manner and represents a complementary approach to traditional methylene forming strategies.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Huiling Liu,Jinglong Han,Jili Yuan,Chengbin Liu,Dong Wang,Tian Liu,Meijun Liu,Jinming Luo,Aijie Wang,John C. Crittenden
Efficient elimination of antibacterial activity of halogenated antibiotics by dehalogenation pretreatment is desired for a biochemical treatment process. In this study, crystalline cobalt phosphide nanosheet arrays on a Ti plate (C-CoP/Ti) are fabricated by a simple electrodeposition and phosphorization process. The crystalline structure greatly promotes atomic hydrogen (H*) generation. Moreover, the nanosheet arrays can provide abundant active sites and accelerate electron transfer and mass transport. As a result, the dehalogenation rate of florfenicol (FLO, an emerging organic pollutant) on C-CoP/Ti is 11.1, 2.97, and 13.6 times higher than that on amorphous CoP/Ti, Pd/Ti, and bare Ti, respectively. The C-CoP/Ti electrode achieves 97.4% dehalogenation of FLO (20 mg L–1) within 30 min at −1.2 V (vs Ag/AgCl). Nearly 100% of Cl and 20% of F are broken away within 120 min, showing the highest electrocatalytic defluorination efficiency reported so far. Both experimental results and theoretical calculations reveal that the dehalogenation of FLO on C-CoP/Ti is synergistically accomplished via direct reduction of electron transfer and indirect reduction of H*. This study develops a highly efficient non-noble metal electrode material for dehalogenation of halogenated organic compounds.
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Frontiers in Chemistry
·
2020
·
IF 3.693
Wang Xiaodong,Hu Weizhao,Hu Yuan
In this study, h-BN@PDA@TiO2 hybrid nanoparticles were prepared and used as functional fillers to prepare PVA nanocomposites, and the effects of hybrid particles on PVA thermal conductivity and flame retardant properties were studied. The results showed that hybrid particles could significantly improve the thermal conductivity and flame retardant performance of PVA composites, and effectively inhibit the release of toxic gases such as combustible pyrolysis products and CO, which enhanced the fire safety of PVA composites. When the addition amount of hybrid particles is 5 wt%, the thermal conductivity of PVA composites is 239.1% higher than that of the pure PVA and the corresponding temperature of PVA composites with a mass loss of 5 wt% was 16.2°C higher than that of the pure PVA. This is due to the barrier effect of h-BN and the protective effect of dense carbon layer catalyzed by TiO2.
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TETRAHEDRON
·
2018
·
IF 2.377
Jie Zhu,Wenhui Zhu,Ping Xie,Charles U. Pittman,Aihua Zhou
A novel and efficient Ni-catalyzed aryl- and alkyl-selenation of imidazo[1,2-α]pyridines employing selenium powder has been developed for the first time. The significant advantages of this protocol are that it is an inexpensive nickel catalyst and exhibits broad functional-group compatibility and good reaction yields.
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Energy Storage Materials
·
2018
·
IF 0
Xu Huang,Xuezhang Xiao,Xuancheng Wang,Zhendong Yao,Chuntao Wang,Xiulin Fan,Lixin Chen
Li-Mg-B-H system with the composition of 2LiBH 4 -MgH 2 is one of the most promising reversible hydrogen storage materials because of the extremely high hydrogen storage capacity (11.5 wt%). Yet, sluggish kinetics with high desorption temperature (~ 400 °C) hindered its practical applications. Herein, a highly efficient catalyst of nanoNi@g-C 3 N 4 , comprised of transition metal nanocatalyst and carbon-based nonmetal material, was designed and fabricated to dramatically reduce its initial hydrogen desorption temperature to as low as ~105 °C, and eliminate induction period between the two dehydrogenation steps of 2LiBH 4 -MgH 2 by reducing the activation energy for the dehydrogenation of LiBH 4 from 200±6 to 126±7 kJ/mol. Multiple postmortem analyses revealed that the in situ formed MgNi 3 B 2 NPs and the H + defects on g-C 3 N 4 play the key role in synergically enhancing the hydrogen reversible desorption/absorption kinetics at low temperature: 1) in situ formed MgNi 3 B 2 acts as nucleation center of MgB 2 and leads to an excellent catalytic effect to accelerate the dehydrogenation kinetics of 2LiBH 4 -MgH 2 ; 2) the H + defects on g-C 3 N 4 , will interact with the H – in LiBH 4 to trigger the release of H 2 at low temperature and destabilize LiBH 4 and MgH 2 to form Li 3 N and Mg 3 N 2 respectively for the high electronegativity of N: 3) these in situ formed intermediates of Li 3 N and Mg 3 N 2 will be readily rehydrogenated as highly reversible Mg(NH 2 ) 2 and LiH. This novel transition metal and g-C 3 N 4 catalytic composites could provide alternative insights into designing nanosized catalytic hydrogen storage system with low desorption temperature and high capacity for hydrogen-fueled applications.
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INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Qi Zhang,Minghui Li,Zhuofan Zuo,Tianhang Zhan,Xiaoyan Li,Wei Zhang
Cotton, as one of the world’s most crucial economic crops, suffers from a markedly shortened service life of its fabrics due to microbial degradation. In this study, N-isopropylacrylamide (NIPAM) containing amide bonds was grafted onto cotton fibers via atom transfer radical polymerization (ATRP) to develop a heat-resistant and wash-durable N-halamine functionalized cotton fabric (PN@CF-Cl). The resulting material exhibited rapid and potent antibacterial activity, killing over 85 % of bacteria within 1 min of contact and achieving > 99.9 % inactivation of Staphylococcus aureus and Escherichia coli within 10 min. After 50 washing cycles at 75 °C, the antibacterial activity retention remained above 97 %. Following storage for 30 days, rechlorination restored the active chlorine content to its initial level. Even after 10 consecutive chlorination–reduction cycles, the active chlorine recovery reached 98.9 %. In addition, the fabric demonstrated high hydrophobicity, air permeability, and moisture vapor transmission. Molecular dynamics (MD) simulations further validated the dynamic interconversion between N–Cl and N–H in the material, elucidating the underlying mechanism for its regenerative performance. Functionalized cotton fabrics based on the N–Cl/N–H dynamic cycling mechanism can extend product lifespan and hold significant promise for applications in medical protective equipment and smart home textiles.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Fan Fan,Hao Xiu,Huiting Ma,Yuting Wang,Yongpeng Cui,Wenqing Yao,Yajun Wang
Efficient separation and rapid migration of photogenerated charges are crucial for achieving high photocatalytic H₂O₂ production. In this study, a K, P, and O co-doped carbon nitride (KPOCN- x ) was synthesized through simple one-pot polymerization for efficient photocatalytic H₂O₂ production. The synergistic doping of metal and non-metal elements enhances light absorption and simultaneously promotes both in-plane and interplane photogenerated charge transfer. Induced by multi-heteroatom doping, especially the form of K bridging, the built-in electric field of KPOCN-5 increases up to 2.27 times that of undoped polymeric carbon nitride (Bulk CN), facilitating the efficient separation of photogenerated charges. Meanwhile, the rod-shaped structure shortens the migration distances of photogenerated charges, further promoting electron transfer and minimizing recombination. As a result, the H₂O₂ production rate of KPOCN-5 reached 3306.6 μmol g −1 h −1 under visible light, approximately 50 times higher than that of Bulk CN. This work highlights the construction of a giant built-in electric field as a powerful strategy for boosting the photocatalytic production of H₂O₂.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2018
·
IF 4.514
Wei Cai,Wenwen Guo,Ying Pan,Junling Wang,Xiaowei Mu,Xiaming Feng,Bihe Yuan,Bibo Wang,Yuan Hu
The potential prospect of hexagonal boron nitride (h-BN) in the fields of polymer composites is severely limited by undesirable exfoliation efficiency and chemical inertness. Herein, bio-based dopamine was employed toward exfoliating bulk h-BN with hydrogen bond action and imparting a highly-active surface. With assistance of polypodamine, SnO 2 nanoparticles were in-situ synthesized and strengthened the interfacial interaction between h-BN and epoxy (EP) matrix. The integrated function of metal oxide/h-BN toward flame retardant and smoke suppression of polymer materials was firstly studied and obtained, in term of reduced peak heat release rate (decreased by 41.1%), lower total heat release (decreased by 30.1%), and suppressed total smoke production (decreased by 21.6%). In addition, the mechanism for enhancements on flame retardant and smoke suppression of EP composites was systematically investigated. Such a design route simultaneously achieves the exfoliation and functionalization of h-BN, thus offering an active platform for further functionalization modification.
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MATERIALS LETTERS
·
2022
·
IF 3.574
Feifei Zhou,Ganghua Pan,Haining Meng,Hailong Sun
For preparing finer and well-dispersed calcium-silicate-hydrate (C-S-H) seeds at a lower cost, the waste solution of acid treatment of recycled concrete aggregates (RCAs) and black liquor from pulping were used for the synthesis of C-S-H seeds. The results show that C-S-H seeds can be successfully fabricated by chemical co-precipitation reaction using the two waste solutions. Interestingly, it was globular rather than traditional foil-like. Furthermore, C-S-H seeds synthesized using the two waste solutions had smaller particle size and better dispersibility. More importantly, it had a more prominent accelerating effect to the strength development of mortar, significantly enhancing the early and long-term compressive strength of mortar.
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CRYSTENGCOMM
·
2022
·Vol. 24
·期 46
·8060-8069
·
IF 3.756
Shu-Qin Qin,Wei Xu,Wen-Cai Ye,Ren-Wang Jiang
Guanidinium–naphthalenedisulfonic acid (GNPS) was used as a molecular catcher because (i) it contains a cavity and channel in the network; (ii) NH2+ can be used as a hydrogen bond donor, and SO3− can be used as a hydrogen bond acceptor; (iii) the co-planar naphthalene rings can form aromatic interactions with guest molecules. The liquid guests 1–8 [(−)-isopulegol (1), (−)-menthyl acetate (2), isoeugenol (3), 2,6-dimethylaniline (4), methyleugenol (5), 2,6-diisopropylaniline (6), methyl salicylate (7) and L(−)-carvone (8)] are successfully encapsulated in the cavity of GNPS and eight new crystals were obtained. Both aromatic and non-aromatic molecules form hydrogen bonds and C–H⋯π interactions with GNPS. Co-crystallization of 1–4 with GNPS led to stronger C–H⋯π interactions as compared to the previously reported GBPS. Furthermore, compounds 5–8 which were not co-crystallized with GBPS were found to be encapsulated in the cavity of GNPS. We found that the aromatic cavity of GNPS with hydrogen bonding and enhanced C–H⋯π interactions can be regarded as a useful tool for the structural determination of liquid molecules. Furthermore, the correct absolute configurations of 1, 2 and 8 can be assigned based on the small Flack parameters because of the presence of sulfur atoms in the host molecule GNPS.
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Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 10
·1-10
·
IF 4.3
Jia Hongwei,Yue Xiaoyang,Hou Yuying,Huang Fei,Cao Cuiyao,Jia Feifei,Liu Guanhua,Zheng Xiaobing,Liu Yunting,Jiang Yanjun
Unspecific peroxygenases exhibit high activity for the selective oxyfunctionalization of inert C(sp 3 )-H bonds using only H 2 O 2 as a clean oxidant, while also exhibiting sensitivity to H 2 O 2 concentration. CdS-based semiconductors are promising for the photosynthesis of H 2 O 2 owing to their adequately negative potential for oxygen reduction reaction via a proton-coupled electron transfer process, however, they suffer from fast H 2 O 2 decomposition on the surface of pristine CdS. Therefore, [Cp*Rh(bpy)H 2 O] 2+ , a highly selective proton-coupled electron transfer catalyst, was anchored onto a supramolecular polymer-grafted CdS nanoflower to construct an efficient integrated photocatalyst for generating H 2 O 2 , mitigating the surface issue of pristine CdS, increasing light absorption, accelerating photonic carrier separation, and enhancing oxygen reduction reaction selectivity to H 2 O 2 . This photocatalyst promoted the light driven H 2 O 2 generation rate up to 1345 µmol·L −1 ·g −1 ·h −1 , which was 2.4 times that of pristine CdS. The constructed heterojunction photocatalyst could supply H 2 O 2 in situ for nonspecific peroxygenases to catalyze the C-H oxyfunctionalization of ethylbenzene, achieving a yield of 81% and an ee value of 99% under optimum conditions. A wide range of substrates were converted to the corresponding chiral alcohols using this photo-enzyme catalytic system, achieving the corresponding chiral alcohols in good yield (51%–88%) and excellent enantioselectivity (90%–99% ee).
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