Catalysis Science & Technology
·
2024
·Vol. 14
·期 6
·1568-1578
·
IF 4.4
Qifeng Chen,Peng Zheng,Haodi Liu,Yuanrong Zhang,Shuaitao Li,Hongpian Guo,Yanfen Fang,Xun Hu,Ran Duan
The combination of photocatalytic dehalogenation of halogenated aromatics and C–C coupling synthesis of valuable organics is an interesting method for the elimination of pollutants and synthesis of valuable chemicals. Herein, we present a green method for the photocatalytic dehalogenation of benzyl bromide and selective coupling synthesis of bibenzyl achieved on the dual active sites of single-atom Cu and surface oxygen vacancies (VOS) generated in situ on ultrathin 2D-TiO2(B) nanosheets. The experimental results show that single-atom Cu sites on ultrathin TiO2(B) nanosheets can improve charge transfer and separation efficiency and stabilize VOS formed in situ; the presence of VOS not only improves light absorption capacity but also favors the adsorption of reactant benzyl bromide molecules. More importantly, the dual sites of single-atom Cu and adjacent VOS form a solid frustrated Lewis pair, favor the adsorption of benzyl bromide molecules, activate the C–Br bond, and boost the C–C coupling synthesis of bibenzyl. This work provides a novel insight into photocatalytic C–C coupling through the synergistic effect of single-atom Cu and VOS on ultrathin nanosheet photocatalysts.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2012
·
IF 2.237
Xiao Chen,Miao Li,Jingchao Guan,Xinkui Wang,Christopher T. Williams,Changhai Liang
Nickel–silicon intermetallics have been prepared by a direct silicification method using SiH4 as the silicon source. The prepared nickel–silicon intermetallics were characterized by X-ray diffraction, transmission electron microscopy, temperature-programmed reduction, temperature-programmed desorption, X-ray photoelectron spectroscopy, and CO chemisorption measurements. The catalytic hydrogenation of cinnamaldehyde and phenylacetylene over the nickel–silicon intermetallics was investigated. Nickel–silicon intermetallics presented much higher selectivity to the intermediate product (hydrocinnamaldehyde) than monometallic nickel catalyst, which may be attributed to the repulsive force between the electronegative silicon atoms in the nickel–silicon intermetallics and oxygen atoms in the C═O bond of cinnamaldehyde. In addition, nickel–silicon intermetallics showed excellent selectivity for the hydrogenation of phenylacetylene to styrene (ca. 93%) due to the strong modification of the electronic structure derived from the interaction of nickel and silicon.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Ni Feng,Caiyan Gao,Cun-Yue Guo,Guangming Chen
We report flexible films of organic–inorganic thermoelectric (TE) composites based on organometallic coordination compound [copper-phenylacetylide (PhC2Cu)] nanobelts and single-walled carbon nanotubes (SWCNTs). Interestingly, an unusual mechanochromic luminescence phenomenon from bright green to dark red is clearly observed after grinding the PhC2Cu crystalline nanobelts. The PhC2Cu/SWCNT composites display high mechanical flexibility and excellent TE performance. The maximum power factor at room temperature can reach as high as 200.2 ± 10.9 μW m–1 K–2. The present study opens an avenue to fabricate novel organic–inorganic TE composite materials using organometallic coordination compounds such as PhC2Cu.
研究领域:
材料科学
·
有机无机复合材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemCatChem
·
2016
·Vol. 8
·期 6
·1111-1118
·
IF 4.724
Xinlin Li,Wei Zhang,Yansheng Liu,Rong Li
Graphical Magnetic personality : A new magnetic porous carbon derived from metal–organic framework is synthesized through the direct carbonization of ZIF-67 crystals and utilized as a support for Pd nanocatalysts. The catalysts are tested in the semihydrogenation of phenylacetylene under extremely mild conditions. A new magnetic porous carbon (MDPC) derived from metal–organic frameworks (MOFs) was synthesized successfully through the direct carbonization of ZIF-67 crystals and utilized as a support for Pd nanocatalysts. The prepared MDPC not only retains the original morphology of ZIF-67 crystals but also provides a high surface area and excellent magnetic properties. The designed catalysts (Pd-MDPC) were tested in the semihydrogenation of phenylacetylene under extremely mild conditions. The Pd nanoparticles are highly dispersed on the MDPC matrix without aggregation and exhibited an excellent catalytic activity and high selectivity toward olefins under mild conditions (25 °C, H 2 1 atm). The Pd-MDPC catalysts were further investigated in the semihydrogenation of several other terminal alkynes. Compared with most traditional carbon materials, such as activated carbon and carbon nanotubes, the MDPC possesses an admirable magnetism so that it could be separated magnetically from the reaction system. Our study indicates that MOF-derived porous carbon is a suitable support for noble-metal nanocatalysts and has promise in the field of nanocatalysis.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL SCIENCES
·
2024
·Vol. 136
·期 1
·1-9
·
IF 1.7
Zhang Mingyu,Yan Dong,Xu Rui,Tang Yuqi,Xu Shuangping,Qu Yanqing,Xu Jingyu,Du Boyu,Jia Hongge
A new rhodium complex [Rh(cod)(TTT) 2 ] was synthesized by [Rh(cod)Cl] 2 as a precursor, and 4,4',4''-(1,3,5-triazine-2,4,6-triyl)trianiline (TTT) as a ligand. Its structure was verified by 1 H and 13 C NMR. The results indicate that the complex shows high activity in phenylacetylene polymerization. It was applied to the polymerization of phenylacetylene with a yield of 45.0% and Mw = 2.26×10 5 at ultra-low rhodium feed ratio ([Rh.]/[M.]=1/60000). Graphical abstract A new rhodium complex [Rh(cod)(TTT) 2 ] was synthesized by [Rh(cod)Cl] 2 as a precursor, and 4,4',4''-(1,3,5-triazine-2,4,6-triyl)trianiline (TTT) as a ligand. It was applied to the polymerization of phenylacetylene with a yield of 45.0% and Mw = 2.26×10 5 at ultra-low rhodium feed ratio ([Rh.]/[M.]=1/60000
研究领域:
无机化学
·
有机金属化学
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高分子化学
·
催化
✓ 已验证
DOI
高影响因子
ELECTROANALYSIS
·
2012
·Vol. 24
·期 2
·286-292
·
IF 2.872
Chengxiang Ruan,Li Xu,Xiuzhen Wang,Jin Lou,Weimin Gao,Wei Sun
In this paper a molecular wire modified carbon paste electrode (MW-CPE) was firstly prepared by mixing graphite powder with diphenylacetylene (DPA). Then a graphene (GR) and chitosan (CTS) composite film was further modified on the surface of MW-CPE to receive the graphene functionalized electrode (CTS-GR/MW-CPE), which was used for the sensitive electrochemical detection of adenosine-5′-triphosphate (ATP). The CTS-GR/MW-CPE exhibited excellent electrochemical performance and the electrochemical behavior of ATP on the CTS-GR/MW-CPE was carefully studied by cyclic voltammetry with an irreversible oxidation peak appearing at 1.369 V (vs. SCE). The electrochemical parameters such as charge transfer coefficient ( α ) and electrode reaction standard rate constant ( k s ) were calculated with the results of 0.53 and 5.28×10 −6 s −1 , respectively. By using differential pulse voltammetry (DPV) as detection technique, the oxidation peak current showed good linear relationship with ATP concentration in the range from 1.0 nM to 700.0 µM with a detection limit of 0.342 nM (3 σ ). The common coexisting substances, such as uric acid, ascorbic acid and guanosine-5′-triphosphate (GTP), showed no interferences and the modified electrode was successfully applied to injection sample detection.
研究领域:
分析化学
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
POLYMERS FOR ADVANCED TECHNOLOGIES
·
2018
·Vol. 29
·期 11
·2797-2805
·
IF 2.137
Hanyuan Li,Wei Wang,Guofei Chen,Xiaoqi Chen,Yantao Li,Haijun Zhou,Xingzhong Fang
Novel highly soluble phenylethynyl-endcapped oligoimides with different calculated molecular weights were prepared by using mellophanic dianhydride and bis(4-amino-2-trifluoromethylphenyl)ether in the presence of 4-phenylethynyl phthalic anhydride as the reactive endcapping agent. The effect of molecular weights of the aromatic oligoimides on their solubility and processability as well as the thermal and mechanical properties of the thermal-cured polyimides was fully investigated. This kind of phenylethynyl-terminated imides exhibited excellent comprehensive properties. Most importantly, a big progress has been made in the solubility of the oligoimides in this paper. Most of the oligoimides showed excellent solubility (more than 33 wt%) even in acetone , which was reported for the first time. And oligoimides with appropriate molecular weights also showed very good processability with minimum melt viscosities no higher than 120 Pa·s by the rheological study. After thermally curing at 370°C for 1 hour, the cured flexible films showed very high glass transition temperatures up to 392°C by dynamic mechanical analysis, and the temperature of 5% weight loss was higher than 500°C in both air and N 2 atmosphere by thermogravimetric analysis. The cured films also exhibited very good toughness with elongation up to 9%.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nanomaterials
·
2021
·Vol. 11
·期 11
·2776
·
IF 5.076
Yuan Huang,Haoting Yan,Chenyang Zhang,Yize Wang,Qinhong Wei,Renkun Zhang
Metal-supported catalyst with high activity and relatively simple preparation method is given priority to industrial production. In this work, this study reported an easily accessible synthesis strategy to prepare Mott-Schottky-type N-doped carbon encapsulated metallic Co (Co@Np+gC) catalyst by high-temperature pyrolysis method in which carbon nitride (g-C3N4) and dopamine were used as support and nitrogen source. The prepared Co@Np+gC presented a Mott-Schottky effect; that is, a strong electronic interaction of metallic Co and N-doped carbon shell was constructed to lead to the generation of Mott-Schottky contact. The metallic Co, due to high work function as compared to that of N-doped carbon, transferred electrons to the N-doped outer shell, forming a new contact interface. In this interface area, the positive and negative charges were redistributed, and the catalytic hydrogenation mainly occurred in the area of active charges. The Co@Np+gC catalyst showed excellent catalytic activity in the hydrogenation of phenylacetylene to styrene, and the selectivity of styrene reached 82.4%, much higher than those of reference catalysts. The reason for the promoted semi-hydrogenation of phenylacetylene was attributed to the electron transfer of metallic Co, as it was caused by N doping on carbon.Keywords:cobalt catalyst;N-doped carbon;Mott-Schottky effect;catalytic hydrogenation;phenylacetylene
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Zhichang Bao,Lei Yang,Zhenmin Cheng,Zhiming Zhou
A non-noble NiZn3/α-Al2O3 catalyst was prepared by a urea co-precipitation method, which showed good stability and high selectivity to styrene (ST) (92% selectivity at above 99% conversion of phenylacetylene (PA)). The high selectivity was mainly attributed to the electronic effect of the Ni–Zn alloy. The selective hydrogenation of the C8 aromatic fraction on NiZn3/α-Al2O3 was well described by a Langmuir–Hinshelwood-type kinetic model. The estimated activation energies for the hydrogenation reactions of PA → ST, ST → ethylbenzene (EB), and PA → EB were 70.31, 81.65, and 74.88 kJ/mol, respectively. A reactor model allowing for an intraparticle diffusion-reaction and external mass transfer was further developed to describe the selective hydrogenation of the C8 aromatic fraction on larger NiZn3/α-Al2O3 particles in a fixed-bed reactor. The observed changes in product composition with the reaction conditions were well predicted by the model, and the results demonstrated that phenylacetylene can be completely removed without loss of styrene under certain conditions.
研究领域:
化学工程
·
催化化学
✓ 已验证
DOI
高影响因子
HETEROCYCLIC COMMUNICATIONS
·
2022
·Vol. 28
·期 1
·149-156
·
IF 2
Rui Xu,Mingyu Zhang,Yuyan Zhang,Hongge Jia
Three novel rhodium complexes, with l -tyrosine ( l -Tyr), l -arginine ( l -Arg), or 2,4-diamino-6-phenyl-1,3,5-triazine (Dpt) as a ligand, named as [Rh(cod)( l -Tyr)], [Rh(cod)( l -Arg)], and [Rh(cod)(Dpt) 2 ], respectively, had been synthesized for catalyzing the polymerization of phenylacetylene. Their yields were 62.34, 54.87, and 58.21%, respectively, by the most suitable synthesis conditions at 25°C for 4 h. The structures and purity of these complexes were proved by 1 H NMR, element analysis, and scanning electron microscope (SEM). It has been examined that phenylacetylene could be polymerized by the three complexes as catalysts with high degrees of polymerization ( n = 368, 385, and 664, respectively) and yields (about 87.62, 88.39, and 59.67%, respectively). In conclusion, compared with traditional [Rh–N] type catalysts, the novel [N–Rh–N] type catalyst ([Rh(cod)(Dpt) 2 ]) gained better catalytic performance. By comparing the yield, Mw, and degree of their polymerization, the polymerization mechanism was found under the [N–Rh–N] type rhodium catalyst system.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Huibin Liu,Wenhao Yang,Weilin Shen,Ying Zhong,Wenjun Zhu,Xiao Chen,Changhai Liang
The long-term scientific challenge and pursuit for semi-hydrogenation of alkynes to alkenes can be satisfied by regulating metal active centers or developing new catalytic materials. Herein, Al-Co x intermetallic catalysts are successfully prepared by reducing metal oxides using LiCl-CaH 2 composite molten salts, which are utilized for the semi-hydrogenation of phenylacetylene to styrene. The AlCo intermetallic catalyst with amorphous alumina encapsulation, resulting from the non-stoichiometric ratio feeding, exhibits significantly high styrene selectivity (83 %) at 99 % conversion of phenylacetylene under 100 °C and 0.3 MPa H 2 , which is much better than those of surface Co-rich samples and Co/Al 2 O 3 catalyst. The selectivity enhancement in phenylacetylene semi-hydrogenation is attributed to the alteration in the adsorption mode of styrene over AlCo intermetallic catalyst surface, which facilitates by the electron-rich and isolated Co active sites. Moreover, in hydrogenation of alkyne with different functional groups and steric hindrances, the corresponding alkene selectivity is similarly satisfactory, and the catalyst is easy to separate and has a stable structure. This work offers a valuable approach for tailoring the catalytic performance of intermetallic compounds formed by transition metal aluminides, and expanding their potential applications in efficient hydrogenation catalysts.
研究领域:
催化化学
·
材料科学
·
有机合成
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xin Song,Mingyi Li,Jiaqi Xiong,Fangjun Shao,Zhongzhe Wei,Wenjuan Fang,Jianguo Wang
The carboxylation of alkynes with CO 2 is a pivotal reaction in organic synthesis. However, the generally poor adsorption and activation of CO 2 in heterogeneous catalytic systems have become a bottleneck problem restricting the efficiency of carboxylation reactions. In this study, we proposed a strategy for modifying heterogeneous catalysts with ionic liquid. By utilizing amino acid ionic liquids to modify the Pd/In 2 O 3 catalyst, the electronic structure of palladium (Pd) nanoparticles is optimized, and the adsorption and activation of CO 2 on the catalyst is enhanced. Additionally, the h-In 2 O 3 support not only regulates the electronic structure of Pd nanoparticles but also provides abundant oxygen vacancies, which facilitates the adsorption of CO 2 in the system. Due to the synergistic catalytic effects of the amino acid ionic liquid and the oxygen vacancies in the h-In 2 O 3 support, the Pd/h-In 2 O 3 -BmimPro catalyst demonstrates a remarkable phenylpropiolic acid yield of 93 % under mild conditions (50 °C, 0.5 MPa). This study provides valuable insights into the application of ionic liquid-modified catalysts in CO 2 conversion technologies.
研究领域:
催化化学
·
有机合成
·
二氧化碳利用
·
材料化学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）