作者机构:
[Nguyen, Nhat Truong; Mao, Chengliang; Duchesne, Paul N.; Wang, Lu; Jelle, Abdinoor A.; Xia, Meikun; Ozin, Geoffrey A.] Univ Toronto, Dept Chem, Solar Fuels Grp, Toronto, ON M5S 3H6, Canada.;[Wang, Lu] Chinese Univ Hong Kong, Sch Sci & Engn, Shenzhen 518172, Guangdong, Peoples R China.;[Mao, Chengliang] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Yan, Tingjiang] Qufu Normal Univ, Coll Chem & Chem Engn, Key Lab Life Organ Anal, Qufu 273165, Shandong, Peoples R China.;[Lu, Zheng-Hong; Li, Peicheng] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON M5S 3E4, Canada.
通讯机构:
[Ozin, Geoffrey A.] U;Univ Toronto, Dept Chem, Solar Fuels Grp, Toronto, ON M5S 3H6, Canada.
关键词:
CO2 photocatalysis;titanium nitride;indium oxide;photothermal;reverse water gas shift
摘要:
Herein is developed a ternary heterostructured catalyst, based on a periodic array of 1D TiN nanotubes, with a TiO(2) nanoparticulate intermediate layer and a In(2)O(3-x)(OH)(y) nanoparticulate shell for improved performance in the photocatalytic reverse water gas shift reaction. It is demonstrated that the ordering of the three components in the heterostructure sensitively determine its activity in CO(2) photocatalysis. Specifically, TiN nanotubes not only provide a photothermal driving force for the photocatalytic reaction, owing to their strong optical absorption properties, but they also serve as a crucial scaffold for minimizing the required quantity of In(2)O(3-x)(OH)(y) nanoparticles, leading to an enhanced CO production rate. Simultaneously, the TiO(2) nanoparticle layer supplies photogenerated electrons and holes that are transferred to active sites on In(2)O(3-x)(OH)(y) nanoparticles and participate in the reactions occurring at the catalyst surface.
作者:
Nguyen, Nhat Truong;Yan, Tingjiang*;Wang, Lu;Loh, Joel Yi Yang;Duchesne, Paul N.;...
期刊:
Small,2020年16(49):2005754- ISSN:1613-6810
通讯作者:
Yan, Tingjiang;Ozin, Geoffrey A.
作者机构:
[Ghoussoub, Mireille; Yan, Tingjiang; Ozin, Geoffrey A.; Nguyen, Nhat Truong; Mao, Chengliang; Wang, Lu; Duchesne, Paul N.; Jelle, Abdinoor A.; Xia, Meikun] Univ Toronto, Dept Chem, Solar Fuels Grp, 80 St George St, Toronto, ON M5S 3H6, Canada.;[Yan, Tingjiang] Qufu Normal Univ, Coll Chem & Chem Engn, Key Lab Lifeorgan Anal, Qufu 273165, Shandong, Peoples R China.;[Lu, Zheng-Hong; Loh, Joel Yi Yang; Kherani, Nazir P.; Li, Pei-Cheng] Univ Toronto, Dept Mat Sci & Engn, 184 Coll St,Suite 140, Toronto, ON M5S 3E4, Canada.;[Mao, Chengliang] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Yan, TJ; Ozin, GA] U;[Yan, Tingjiang] Q;Univ Toronto, Dept Chem, Solar Fuels Grp, 80 St George St, Toronto, ON M5S 3H6, Canada.;Qufu Normal Univ, Coll Chem & Chem Engn, Key Lab Lifeorgan Anal, Qufu 273165, Shandong, Peoples R China.
关键词:
CO 2 photocatalysis;indium oxide;photothermal;plasmon resonance;titanium nitride
摘要:
<jats:title>Abstract</jats:title><jats:p>Nanoscale titanium nitride TiN is a metallic material that can effectively harvest sunlight over a broad spectral range and produce high local temperatures via the photothermal effect. Nanoscale indium oxide‐hydroxide, In<jats:sub>2</jats:sub>O<jats:sub>3−</jats:sub><jats:italic><jats:sub>x</jats:sub></jats:italic>(OH)<jats:italic><jats:sub>y</jats:sub></jats:italic>, is a semiconducting material capable of photocatalyzing the hydrogenation of gaseous CO<jats:sub>2</jats:sub>; however, its wide electronic bandgap limits its absorption of photons to the ultraviolet region of the solar spectrum. Herein, the benefits of both nanomaterials in a ternary heterostructure: TiN@TiO<jats:sub>2</jats:sub>@In<jats:sub>2</jats:sub>O<jats:sub>3−</jats:sub><jats:italic><jats:sub>x</jats:sub></jats:italic>(OH)<jats:italic><jats:sub>y</jats:sub></jats:italic> are combined. This heterostructured material synergistically couples the metallic TiN and semiconducting In<jats:sub>2</jats:sub>O<jats:sub>3−</jats:sub><jats:italic><jats:sub>x</jats:sub></jats:italic>(OH)<jats:sub>y</jats:sub> phases via an interfacial semiconducting TiO<jats:sub>2</jats:sub> layer, allowing it to drive the light‐assisted reverse water gas shift reaction at a conversion rate greatly surpassing that of its individual components or any binary combinations thereof.</jats:p>
作者:
Mao, Chengliang;Wang, Jiaxian;Zou, Yunjie;Qi, Guodong;Loh, Joel Yi Yang;...
期刊:
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2020年142(41):17403-17412 ISSN:0002-7863
通讯作者:
Zhang, Lizhi;Ozin, Geoffrey A.
作者机构:
[Zhang, Lizhi; Zou, Yunjie; Liu, Xiao; Ai, Zhihui; Wang, Jiaxian; Mao, Chengliang; Shang, Huan; Zhao, Jincai; Li, Jie; Li, Meiqi] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Ghoussoub, Mireille; Mao, Chengliang; Wang, Lu; Xia, Meikun; Ozin, Geoffrey A.] Univ Toronto, Dept Chem, Solar Fuels Cluster, Mat Chem & Nanochem Res Grp, Toronto, ON M5S 3H6, Canada.;[Qi, Guodong; Xu, Jun; Deng, Feng] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math,Innovat Acad Precis Measur, Wuhan 430071, Peoples R China.;[Loh, Joel Yi Yang; Kherani, Nazir P.] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON M5S 3E4, Canada.;[Zhang, Tianhua] Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst NERC C, Sch Chem Engn, Fuzhou 350002, Fujian, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;[Ozin, Geoffrey A.] U;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;Univ Toronto, Dept Chem, Solar Fuels Cluster, Mat Chem & Nanochem Res Grp, Toronto, ON M5S 3H6, Canada.
摘要:
Optimizing kinetic barriers of ammonia synthesis to reduce the energy intensity has recently attracted significant research interest. The motivation for the research is to discover means by which activation barriers of N-2 dissociation and NHz (z = 1-2, surface intermediates) destabilization can be reduced simultaneously, that is, breaking the "scaling relationship". However, by far only a single success has been reported in 2016 based on the discovery of a strong-weak N-bonding pair: transition metals (nitrides)-LiH. Described herein is a second example that is counterintuitively founded upon a strong-strong N-bonding pair unveiled in a bifunctional nanoscale catalyst TiO2-xHy/Fe (where 0.02 <= x <= 0.03 and 0 < y < 0.03), in which hydrogen spillover (H) from Fe to cascade oxygen vacancies (O-V-O-V) results in the trapped form of O-V-H on the TiO2-xHy component. The Fe component thus enables facile activation of N-2, while the O-V-H in TiO2-xHy hydrogenates the N or NHz to NH3 easily.
期刊:
Journal of Thermoplastic Composite Materials,2020年33(6):817-827 ISSN:0892-7057
通讯作者:
Zhang, Yu
作者机构:
[Zhang, Yu; Wang, Liangjie; Weng, Fangqing; Deng, Yinghua; Zhou, Shiyi] Hubei Univ Educ, Coll Chem & Life Sci, Wuhan 430205, Peoples R China.;[Wu, Qiangxian; Weng, Fangqing; Dou, Xiaoya] Cent China Normal Univ, Coll Chem, Green Polymer Lab, Wuhan, Peoples R China.
通讯机构:
[Zhang, Yu] H;Hubei Univ Educ, Coll Chem & Life Sci, Wuhan 430205, Peoples R China.
关键词:
Rubber;Starch;Structure (composition);Styrene;Toughness;Butadiene rubber;compatibility;Composites material;Elongation at break;Good compatibility;Micro-particles;Scanning electron microscopic;Structure and properties;Polyurethanes
摘要:
We prepared a novel covalent rubber-based polyurethane/starch composites material via a simple and effective method. Infrared, scanning electron microscopic, and mechanical tests demonstrated that polyurethane microparticles showed good compatibility with starch as the polyurethane content increases. This is mainly because of the urethane bond newly formed by –OH in starch and –NCO in rubber-based polyurethane. And when the rubber-based polyurethane content increased from 20% to 30%, its elongation at break improved by 116.9%. CPB30 showed excellent hydrophobicity and toughness, which showed potential application.
摘要:
<jats:title>Abstract</jats:title><jats:p>A tandem phospha‐Michael addition/<jats:italic>N</jats:italic>‐acylation/intramolecular Wittig reaction of in situ formed aza‐<jats:italic>o</jats:italic>‐QMs is disclosed. This approach features high functional group tolerance and provides a convenient and practical access to biologically significant indole derivatives (37 examples, up to 91% yield) under mild reaction conditions.</jats:p><jats:p><jats:boxed-text content-type="graphic" position="anchor"><jats:graphic xmlns:xlink="http://www.w3.org/1999/xlink" mimetype="image/png" position="anchor" specific-use="enlarged-web-image" xlink:href="graphic/adsc202000343-toc-0001-m.png"><jats:alt-text>magnified image</jats:alt-text></jats:graphic></jats:boxed-text>
</jats:p>
摘要:
In this work, a relationship between the role of NH3 and the properties of mineral oxides (alpha-Fe2O3, alpha-Al2O3, CaO, and MgO) in the evolution of NO3-, SO42-, and NH4+ has been established. It was found that the promotion effect of NH3 was more favorable for the formation of NO3- (or SO42-) and NH4+ on acidic alpha-Fe2O3 and alpha-Al2O3 due to acid base interactions between NO2 with NH3 or between SO2 and NH3, while this effect was weaker on basic CaO and MgO possibly due to their basic nature. The acid base interaction (NO2/SO2 with NH3) overpowered the redox reaction (SO2 with NO2) on Fe2O3 owing to its unique redox chemistry. However, the opposite was found on basic CaO and MgO for the formation of SO42- and NO3-. Under equivalent concentration conditions, the two synergistic effects did not further strengthen on Fe2O3, CaO and MgO due to a competition effect. In NH3-rich situation, a synchronous increase of SO42-, NO3-, and NH4+ occurred on Fe2O3. On acidic Al2O3, the favorable adsorption of NH3 on the surface as well as the existence of NO2 with an oxidizing capability synergistically promoted the formation of SO42-, NO3-, and NH4+.
摘要:
A new cadmium(II) arenedisulfonate coordination polymer with uncoordinated pyridyl groups, formulating as [Cd(tpim)(2,6-nds)](n) (1), was synthesized by the hydrothermal reaction of 2,6-naphthalenedisulfonate (2,6-nds), 2,4,5-tri(4-pyridyl)-imidazole (tpim) and Cd(CH3COO)(2). The functional utility is investigated by employing 1 as an efficient heterogeneous nucleophilic catalyst for the acetylation of phenols. The catalyst 1 is stable under the studied reaction conditions, and could be recycled without significantly losing activity.
作者机构:
[Wang, Lei; Zhang, Zhe; Li, Xiaopeng] Univ S Florida, Dept Chem, Tampa, FL 33620 USA.;[Liu, Changlin; Zhang, Zhe] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Jiang, Xin; Wang, Ming] Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Jilin, Peoples R China.;[Irvin, Jennifer A.] Texas State Univ, Dept Chem & Biochem, San Marcos, TX 78666 USA.
通讯机构:
[Li, Xiaopeng] U;[Wang, Ming] J;Univ S Florida, Dept Chem, Tampa, FL 33620 USA.;Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Jilin, Peoples R China.
摘要:
The self-assembly behavior of a tritopic 2,2':6',2 ''-terpyridine (tpy) ligand with Cd(II), Zn(II), and Fe(II) has been exploited herein to generate a series of tetrameric and hexameric macrocycles. The main advantage of using such transition metals with an octahedral coordination geometry is their distinct coordination abilities (e.g., binding strength and reversibility). With the same ligand, this study reveals that the supramolecular structural variation between tetrameric and hexameric macrocycle architectures can be precisely controlled using different metal ions with the same coordination geometry. When Cd(II) was used, a tetrameric macrocycle was the only observed structure in the self-assembly, whereas Zn(II) and Fe(II) assembled a mixture of tetrameric and hexameric macrocycles. Because of the high stability of Fe(II) as the coordination center, we successfully isolated tetrameric and hexameric macrocycles using a regular column. In-depth characterization was carried out to establish the proposed structures, including multinudear NMR (H-1, F-19, and C-13) analysis, electrospray ionization mass spectrometry, and 2D ion-mobility mass spectrometry.
摘要:
In this study, an electrochemical/electro-Fenton oxidation (EC/EF) system was designed to degrade atrazine, by utilizing boron-doped diamond (BDD) and Fe@Fe2O3 core-shell nanowires loaded active carbon fiber (Fe@Fe2O3/ACF) as the anode and the cathode, respectively. This EC/EF system exhibited much higher degradation rate, decholorination and mineralization efficiency of atrazine than the electrochemical (EC) and electrochemical/traditional electro-Fenton (EC/TEF) oxidation counterpart systems without Fe@Fe2O3 core-shell nanowires. Active species trapping experiment revealed that Fe@Fe2O3 could activate molecular oxygen to produce more OH through Fenton reaction, which favored the atrazine degradation. High performance liquid chromatography, high performance liquid chromatography-mass spectrometry and gas chromatography-mass spectrometry were applied to probe the decomposition and mineralization of atrazine during this novel EC/EF process, which revealed that two intermediates of triazinons (the isomerization of hydroxylated atrazine) were generated during the electrochemical/electro-Fenton oxidation of atrazine in the presence of Fe@Fe2O3 core-shell nanowires. The experimental and theoretical calculation results suggested that atrazine might be degraded via a triazinon ring opening mechanism, while the presence of Fe@Fe2O3 notably accelerated the decholorination process, and produced more hydroxylated products to promote the generation of trazinons and the subsequent ring cleavage as well as the final complete mineralization. This work provides a deep insight into the triazine ring opening mechanism and the design of efficient electrochemical advanced oxidation technologies (EAOTs) for persistent organic pollutant removal.
摘要:
<jats:p>The catalytic intramolecular Wittig reactions of carbonyl‐containing bromides are reported. The R<jats:sub>3</jats:sub>PO byproducts participate in the catalytic cycle; therefore, the Wittig reaction can be accomplished with only a catalytic amount of organophosphorus reagent. The reaction has also been applied to the efficient and selective synthesis of isoquinolin‐1(2<jats:italic>H</jats:italic>)‐ones, indoles, 2,3‐dihydro‐1<jats:italic>H</jats:italic>‐2‐benzazepin‐1‐ones, benzofurans, and 1,2‐dihydroquinolines with a catalytic amount of phosphine oxide (0.1 equiv.) and a tetramethyldisiloxane/titanium isopropoxide [TMDS/Ti(O<jats:italic>i</jats:italic>Pr)<jats:sub>4</jats:sub>] reductant system (yields: 35–88 %).</jats:p>
作者机构:
[Xiong, Bo; Wang, Lingling; Jiang, Shichang; Wang, Yujiao; Ye, Mingyue; Bao, Yajing] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticides & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Xiong, Bo] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticides & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
A microfluidic emitter based on three-dimensional hydrodynamic focusing was developed to generate a wrapped charged aerosol plume, in which the distribution of the sample ion in the nanoelectrospray could be regulated. Deposition patterns of the wrapped spray from the proposed three-dimensional hydrodynamic focusing nanoelectrospray emitter (3D HFNE) were collected under different conditions to ensure the wrapped configuration. Moreover, sample ion intensities as well as their ratios to a focusing background ion were studied as a function of different displacements from the center of the wrapped electrospray to confirm the inhibition of ion expansion. Furthermore, the proposed 3D HFNE indicated improved sensitivities compared with a reported nanoelectropray emitter as well as its commercial ESI counterpart, and this demonstrated its capacity for determining samples with low concentrations and infusion rates. In addition, the proposed 3D HFNE was compatible with various sample flow compositions (from 100% methanol to 100% water) and a broad infusion rate range (from 10 nL min(-1) to 15 mu L min(-1)). Finally, its stability and durability were indicated to be acceptable for various determinations. Therefore, the 3D HFNE is a potential option to achieve on-line nanoelectrospray MS determinations using microfluidics with conventional mass spectrometers, considering its low cost and user-friendly properties.
期刊:
Journal of Organometallic Chemistry,2016年823:1-7 ISSN:0022-328X
通讯作者:
Xu, Lin
作者机构:
[Wang, Cui-Hong; Chen, Li-Jun; Wang, Lilei; Xu, Lin] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, 3663 N Zhongshan Rd, Shanghai 200062, Peoples R China.;[Tan, Hongwei; Ma, Jian-Qiu] Beijing Normal Univ, Dept Chem, Beijing 100050, Peoples R China.;[Huang, Junhai] China State Inst Pharmaceut Ind, Zhangheng Inst, 1599 Zhangheng Rd, Shanghai, Peoples R China.;[Xiao, Fengping] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Xu, Lin] E;East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, 3663 N Zhongshan Rd, Shanghai 200062, Peoples R China.
关键词:
Electronic properties;Electrospray ionization;Mass spectrometry;Metals;Molecular orbitals;Orbital calculations;Coordination-driven self assembly;Electrochemical;Electrochemical behaviors;Electrochemical studies;Ionization time of flight mass spectrometries;Metallodendrimer;Multiferrocene;Semi-empirical molecular orbital method;Self assembly