RSC Advances
·
2015
·Vol. 5
·期 128
·105747-105752
·
IF 3.84
Yuanyuan Zheng,Xiaoming Zhang,Yi Yao,Xiaohong Chen,Qihua Yang
Ultra-small Au nanoparticles (<2 nm) supported on hollow silica nanospheres were successfully fabricated with the aid of chemical modification (–SH groups) or through simple immersion method, leading to supported catalysts Au/SH-HNS and Au/HNS. The resulting solid catalysts showed good thermal stability and the small particle sizes could be remained even at high temperature of 350 °C. Such catalysts were catalytically active in the oxidation of styrene using O2 as oxidant under 1 atm pressure. The catalytic results showed that the activity strongly depends on the Au loading amount, and the loading of 4–5 wt% led to the highest activity. Significant rate enhancement was observed with gold nanoparticles supported on pure silica in comparison with thiol modified silica nanospheres, suggesting the negative effects of thiol groups. The solid catalyst could be reused at least 8 reaction cycles without significant decrease in activity and selectivity. This study not only supplies an active, recoverable catalyst for the green transformation of styrene, but also demonstrates that the hollow silica nanosphere material has a superior ability in stabilizing metal nanoparticles against growth.
研究领域:
纳米催化
·
材料化学
·
绿色化学
·
有机氧化反应
·
多相催化
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Kai-Wen Cao,Hao Huang,Fu-Min Li,Hong-Chang Yao,Juan Bai,Pei Chen,Pu-Jun Jin,Zi-Wei Deng,Jing-Hui Zeng,Yu Chen
The reactive and stable catalysts for the oxygen reduction reaction are highly desirable for low temperature fuel cells. The commercial oxygen reduction reaction electrocatalysts generally reply on noble metal based nanomaterials, which suffer from inherent cost and selectivity issues. At present, it still remains challenge for designing efficient non-noble metal-based oxygen reduction reaction electrocatalysts. Herein, we successfully synthesize Co nanoparticles supported on three-dimensionally N-doped holey graphene aerogels hybrids by the high-temperature calcination of the graphene aerogels-polyallylamine-Co II hybrids. The component optimized hybrids show the excellent electrocatalytic activity for oxygen reduction reaction in alkaline media, which is comparable to commercial Pt/C electrocatalyst. Meanwhile, the hybrids also show eminent tolerance for CO and methanol, attributing to their excellent oxygen reduction reaction selectivity. The three-dimensionally interconnected structure of graphene aerogels, N-doping, uniform dispersion and high crystallinity of Co nanoparticles, and holey structure of graphene contribute to the striking oxygen reduction reaction activity of hybrids.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源材料
·
燃料电池
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·Vol. 10
·期 6
·108837
·
IF 7.968
Yumei Jian,Ye Meng,Jie Li,Hongguo Wu,Shunmugavel Saravanamurugan,Hu Li
Photocatalytic reductive conversion of bio-derivatives to biofuels and fine chemicals is an eco-friendly and energy-saving way for biomass valorization. Herein, we developed a new and high-performance protocol for control of activity/selectivity in photocatalytic reductive upgrading of biomass to biofuels at room temperature via engineering oxygen vacancy (Ov) and manipulating the exposed crystal surfaces of the TiO 2 -based catalysts, such as efficient cascade photocatalytic hydrogenation-cyclization of ethyl levulinate to γ-valerolactone in water (up to 96% yield, TOF: 112.1 h −1 ), and the selective conversion of 5-methylfurfural to 5-methylfurfuryl alcohol (90% yield) or long carbon-chain coupling products (86% yield) in methanol, respectively. The {101} crystal plane is prone to produce more Ov in situ than the {001} and {110} crystal planes. The formation of Ov was not only beneficial to the adsorption and activation of the bio-based carbonyls, but also could enhance the migration efficiency of the photo-generated carriers and effectively adjust the semiconductor band structure of the TiO 2 -based photocatalyst to promote the visible-light absorption, thus enhancing the overall reductive conversion process, as elucidated by DFT calculations. Also, the charge distribution and adsorption intensity of different exposed crystal surfaces of the photocatalyst were able to control the selectivity of the bioproducts . In addition, the optimal Ov-TiO 2− x {101} catalyst had excellent reusability and could be reused at least five times with no obvious decrease in photocatalytic performance. The strategy of selectivity control via engineering the catalyst exposed crystal surfaces and loaded Ov provides an opportunity for multi-catalytic biomass conversion to biofuels.
研究领域:
催化化学
·
材料科学
·
能源化学
·
环境科学
·
绿色化学
·
表面科学
·
光催化
✓ 已验证
DOI
高影响因子
Green Energy & Environment
·
2019
·Vol. 4
·期 4
·424-431
·
IF 0
Yangyang Zhang,Xinli Tong,Linhao Yu,Lingwu Meng,Pengfei Guo,Song Xue
The catalytic transformation of furfuryl alcohol and hexose into value-added chemicals have been investigated with a series of polymer-based catalysts including poly(styrenesulfonic acid) (PSS), graphite oxide-doped poly(styrenesulfonic acid) (PSS-GO), and graphite-doped poly(styrenesulfonic acid) (PSS-C). It is found that the selective conversion of furfuryl alcohol to methyl levulinate (MLE) was successfully performed with PSS as the catalyst, in which a 96.4% yield is attained in methanol solvent. Moreover, the efficient dehydration of d -fructose to produce 5-hydroxymethylfurfural (HMF) has also been achieved using PSS-GO as the catalyst, where a 76.5% yield of HMF was obtained in N -methylpyrrodinone solvent. The effects of reaction temperature, time and solvent were investigated. Furthermore, the used catalysts have been respectively characterized by XRD, TG, FTIR, SEM and TEM techniques to reveal the physical properties and structures of these polymeric catalytic materials.
研究领域:
催化化学
·
生物质能源
·
绿色化学
·
有机转化
·
高分子材料
·
可持续化学
·
生物基化学品
✓ 已验证
DOI
CARBON
·
2018
·
IF 7.082
Xian Wang,Zuju Ma,Lulu Chai,Leqiong Xu,Ziyi Zhu,Yue Hu,Jinjie Qian,Shaoming Huang
Growing demand for clean and renewable energy resources has sparked intensive research on the development of an effective strategy to prepare non-noble metal electrocatalysts for oxygen evolution reaction (OER). Herein, we report a new type of N-doped carbon coated CoP particle/carbon nanotube composite (CNT-NC-CoP) has been synthesized by in situ nucleation and growth of ZIF-67 nanoparticles onto carbon nanotubes, which subsequently is treated with carbonization and phosphorization. Unique hierarchical structure endows as-obtained CNT-NC-CoP with high specific surface area , abundant exposed active sites, quick ion diffusion path , and good electrical conductivity , thus exhibiting the highest electrocatalytic capability with the low overpotential of 251 mV at the current density of 10 mA cm −2 and remaining long-term durability (overlapping LSV curve after 10 h). Besides, density functional theory (DFT) calculations reveal that CoOOH/graphene charged surfaces are more effective for facilitating intermediates adsorption and improving the corresponding catalytic activity .
研究领域:
材料化学
·
电化学
·
纳米材料科学
·
能源催化
·
功能材料
·
计算材料学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 18
·53492-53504
·
IF 5.8
Tang Hao,Liu Xiaolong,Li Yiren,Tian Jinglei,Hou Changjiang,Tian Mengkui,Zhu Tingyu
Based on the unique technique property of grate–kiln pellet production process and its demand of ultra-low emission of NO x , a low energy-consumed embedded selective catalytic reduction (SCR) denitration technology was proposed. The temperature of the NO x -containing tributary flue gas was 350–500 °C, which basically accorded with the temperature range of SCR by V 2 O 5 -based catalyst. Considering the potential inhibition effect of high SO 2 concentration (8000–10000 mg/m 3 ) and metal-containing dust in the pelletizing flue gas, the catalyst compositions were optimized to V 2 O 5 (0.5%) and WO 3 (5%), giving NO conversion over 90% with low yield of N 2 O by-product. Compared with the low-medium temperature SCR technology, it was no longer necessary to reheat the flue gas, showing a remarkable CO 2 emission reduction effect. The CO 2 emission reduction ratios were 94% and 66% contributed by the decrease of fuel and electricity consumption for the embedded SCR technology, respectively. The operating cost was also greatly reduced from 11.4 CNY/t-pellet to 3.1 CNY/t-pellet (Chinese Yuan).
研究领域:
环境工程
·
大气污染控制
·
化学工程
·
能源与环境科学
·
工业生态学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Zhenzhen Yang,Renliang Huang,Wei Qi,Liping Tong,Rongxin Su,Zhimin He
Reduced graphene oxide functionalized with magnetic Fe 3 O 4 nanoparticles and –PhSO 3 H groups (Fe 3 O 4 -RGO-SO 3 H) was reported for environmentally benign hydrolysis of cellulosic materials, which is an important process in integrated utilization of biomass resource. Except for –PhSO 3 H groups, –COOH and –OH groups derived from graphene oxide (GO) were also expected in the structure of Fe 3 O 4 -RGO-SO 3 H. Fe 3 O 4 -RGO-SO 3 H exhibited outstanding catalytic performance for the hydrolysis of cellulosic materials, due to its crumpling feature with clear layers and the coexistence of –COOH and –OH groups. The unique structure of Fe 3 O 4 -RGO-SO 3 H favors the accessibility of cellulose to the active sites of the material and facilitates the diffusion of the product molecules. –COOH groups on the surface of the material provide a large concentration of acidic functionality for hydrolyzing cellulose, while –OH groups readily adsorb cellulose through forming strong hydrogen bonds between –OH groups and the oxygen atoms in β-1,4 glycosidic bonds. Furthermore, Fe 3 O 4 -RGO-SO 3 H can also be easily separated from the reaction residue with an extra magnetic force and further used at least five times.
研究领域:
材料化学
·
催化化学
·
生物质能源
·
绿色化学
·
纳米材料科学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Kexin Chen,Xi Wang,Pengfei Xia,Jinxin Xie,Jing Wang,Xukai Li,Yiming Tang,Laisheng Li
Z-scheme Cu 2 O-(rGO-TiO 2 ) photocatalyst was successfully synthesized via a simple three-step approach for 2,2′,4,4′-tretrabromodiphenyl ether (BDE47) reductive removal under simulated solar irradiation. Unlike the traditional heterojunction , the addition of reduced graphene oxide (rGO) enhanced the redox ability of Cu 2 O-TiO 2 by increasing charge transfer. When modifying Cu 2 O films by adding 1% rGO and coating with 70% TiO 2 , the resulting Cu 2 O-(rGO-TiO 2 ) exhibited the best photocatalytic activity for BDE47 removal. The charge transfers of Cu 2 O-(rGO-TiO 2 ) were proven to follow a Z-scheme pathway through the electron paramagnetic resonance analysis. The degradation pathways of BDE47 were elucidated by identifying intermediate products via gas chromatography-mass spectrometry (GC-MS) and gas chromatography (GC). Photo-electrons (e − ) generated from the conduction band of Cu 2 O and hydrogen protons (H 0 ) reduced from H + in water were the main contributing elements for the removal of BDE47, which response to the ortho and para debromination . Ortho-Br of BDE47 was attacked by e − and BDE28 was the dominant debromination product on the first stage. Then e − and H 0 attacked ortho-Br and para-Br of BDE28 to form BDE15 and BDE8, respectively. The concentration of BDE8 was higher than that of BDE15, suggesting that H 0 played the most important role on the second debromination stage. An effective Cu 2 O-(rGO-TiO 2 )-based Z-scheme system for BDE47 debromination was proposed in this study, which may contribute to the development of novel green technologies.
研究领域:
环境科学
·
光催化化学
·
环境污染与控制
·
材料科学
·
绿色技术
·
有机污染物降解
✓ 已验证
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 134
·期 46
·45484
·
IF 1.86
Teng Xue,Erjun Tang,Jian Zhou,Ruitao Han,Shaojie Liu
A coordinating ionic liquid (IL), 1-[(diethyl amine)amine]ethyl-3-methyl imidazolium chloride ([N 3 MIM]Cl), was prepared as an alternative to a simple organic ligand to coordinate to copper(I) bromide (CuBr). We, thereby, obtained a novel catalyst for atom transfer radical polymerization (ATRP) reactions. This catalyst was applied to the ATRP of methyl methacrylate in the IL 1-allyl-3-methyl imidazolium chloride ([AMIM]Cl). The chemical structures of the ILs obtained were confirmed by Fourier transform infrared spectroscopy, mass spectrometry, and 1 H-NMR analyses. The coordination ability of [N 3 MIM]Cl was assessed by cyclic voltammetry, and the redox potential of [N 3 MIM]Cl–CuBr was −0.507 V. The [N 3 MIM]Cl–CuBr complex was expected to be a markedly more active catalyst than the amine DETA–CuBr complex. The coordination mode toward CuBr was also examined. The [N 3 MIM]Cl–CuBr catalyst system showed good controllability in the aforementioned ATRP reaction in [AMIM]Cl. The Cu catalyst was easily separated from the obtained polymer with the coordinating IL as a ligand. Consequently, the coordinating IL overcame the shortcomings of traditional organic ligands, such as poor compatibility with IL media and poor separation of the catalyst from the polymer; this makes it highly promising for applications in the ATRP field. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 45484.
研究领域:
高分子化学
·
催化化学
·
功能材料
·
绿色溶剂
·
配位化学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of CO2 Utilization
·
2017
·
IF 4.292
Lijun Zhao,Haiyang Cheng,Tong Liu,Yan Li,Zhong Ying,Wenjing Yang,Weiwei Lin,Xiangchun Meng,Chengxue Wang,Fengyu Zhao
An efficient green process was developed for production of p -aminophenol (PAP) from hydrogenation of nitrobenzene (NB) over a traditional Pt/Al 2 O 3 catalyst in a reaction medium of supercritical CO 2 (scCO 2 ) and H 2 O without any additional acid catalyst involved. The combination of scCO 2 and H 2 O was confirmed to be effective for the production of PAP. The acidity, aroused by the in situ formed carbonic acid, increased with CO 2 pressure, which acted as acid catalysis during the reaction, and it can easily self-neutralize by depressurization of CO 2 , resulting in a green and a intensive process for it removed the final neutralization and salts disposal of the traditional liquid acids. Under the optimal reaction conditions, a high yield to PAP (68.9%) was achieved at the high conversion of NB (98.5%). Moreover, the results of in situ diffuse reflectance FTIR spectra revealed that CO was generated by the reverse water-gas shift reaction (CO 2 + H 2 → CO + H 2 O), it can adsorbed on the surface of Pt/Al 2 O 3 to suppress the undesired deep hydrogenation of N -phenylhydroxylamine (PHA) to aniline (AN), which also contributed to the obtained high selectivity of PAP. Therefore, the present green and efficient catalysis process will arouse the interest of researchers in the fields of the green and sustainable organic synthesis.
研究领域:
绿色化学
·
有机合成
·
催化化学
·
环境友好工艺
·
工业化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2013
·Vol. 1
·期 13
·4228-4235
·
IF 0
Yu Bai,Ran Long,Chengming Wang,Ming Gong,Yanrui Li,Hao Huang,Hui Xu,Zhengquan Li,Mingsen Deng,Yujie Xiong
A method has been developed for controlled epitaxial growth on cubic nanocrystals by selectively activating their surface via etching. For example, it produces Pd concave nanocubes via seeding growth on their corners and edges, and in turn, formulates highly active sites for catalysis. This method offers a better capability of preventing atomic addition on undesired locations and maintaining particle size in the seeding process, as compared with the previous technique. With the particle size well maintained, the products fully exhibit superior electrocatalytic performance enabled by active sites and high-index facets in formic acid oxidation. Another contribution of this work is to enable the growth of a noble metal with high catalytic activities on another type of cheaper metal, which greatly reduces the usage of expensive materials while retaining high catalytic activity. In this article, we have demonstrated the deposition of a very limited amount of Pt (only 3.3 wt%) on Pd nanocrystals towards high electrocatalytic activities in an oxygen reduction reaction. Preliminary studies demonstrate that the synthetic strategy can be also applied to the controllable deposition of a different material on the faces of a nanocrystal by simply altering surface conditions.
研究领域:
材料化学
·
纳米科学与技术
·
催化化学
·
电化学
·
表面科学
·
功能纳米材料
✓ 已验证
DOI
APPLIED ORGANOMETALLIC CHEMISTRY
·
2013
·Vol. 27
·期 3
·148-154
·
IF 2.011
Li Qiang Wu
Nano n -propylsulfonated γ-Al 2 O 3 is easily prepared by the reaction of nano γ-Al 2 O 3 with 1,3-propanesultone. This reagent can be used as an efficient catalyst for the synthesis of spiro [indoline-3,4-pyrazolo[3,4- e ][1,4]thiazepine]diones in aqueous media. This new method consistently has the advantages of excellent yields and short reaction times. Further, the catalyst can be reused and recovered several times. Copyright © 2013 John Wiley & Sons, Ltd.
研究领域:
催化化学
·
有机合成
·
绿色化学
·
纳米材料
·
药物化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）