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| 1 | High population and dispersion of pentacoordinated Al~Ⅴ species on the surface of ?ame-made amorphous silica-alumina显示文摘Pentacoordinated Al(Al~Ⅴ)species in silica-alumina are promising to promote the formation of acid sites or act as surface defects for tailoring single-atom catalysts.However,pentahedral coordination(Al~Ⅴ)is rarely observed in conventionally prepared silica-alumina.Here,we show that high population and dispersion of Al~Ⅴ species on the surface of amorphous silica-alumina(ASA)can be achieved by means of flame spray pyrolysis.High resolution TEM/EDX,high magnetic-field NMR and DFT calculations are employed to characterize the structure of as-prepared ASAs.Solid-state ^(27)Al multi-quantum MAS NMR experiments show that most of the Al~Ⅴspecies are formed independently from the alumina phase and are accessible for guest molecules on the surface.Upon water adsorption,these Al~Ⅴ species are transformed to Al~Ⅵ species,structurally similar to surface Al~Ⅳ species,as confirmed by DFT calculations.The outstanding catalytic activity of as-synthesized ASA is demonstrated using the in situ H/D exchange reaction with deuterated benzene as an example.The Al~Ⅴ-rich ASA provides a much lower activation energy(~30 kJ/mol)than that reported for zeolite H-ZSM-5(~60 kJ/mol).The superior catalytic performance is attributed to the high Al~Ⅴcontent promoting the surface active sites in ASA.The knowledge gained on the synthesis of Al~Ⅴ-rich ASAs and the nature of aluminum coordination in these materials could pave the way to more efficient silica-alumina based catalysts. | Zichun Wang Yijiao Jiang Xianfeng Yi Cuifeng Zhou Aditya Rawal James Hook Zongwen Liu Feng Deng Anmin Zheng Michael Hunger Alfons Baiker Jun Huang | 2019 | Science Bulletin2019，64，8： | 2 |
| 2 | Continuous dimethyl carbonate synthesis from CO_(2) and methanol over Bi_(x)Ce_(1-x)O_(δ) monoliths:Effect of bismuth doping on population of oxygen vacancies,activity,and reaction pathway显示文摘We evaluated bismuth doped cerium oxide catalysts for the continuous synthesis of dimethyl carbonate(DMC)from methanol and carbon dioxide in the absence of a dehydrating agent.Bi_(x)Ce_(1-x)O_(δ)nanocomposites of various compositions(x=0.06-0.24)were coated on a ceramic honeycomb and their structural and catalytic properties were examined.The incorporation of Bi species into the CeO_(2) lattice facilitated controlling of the surface population of oxygen vacancies,which is shown to play a crucial role in the mechanism of this reaction and is an important parameter for the design of ceria-based catalysts.The DMC production rate of the Bi_(x)Ce_(1-x)O_(δ) catalysts was found to be strongly enhanced with increasing Ov concentration.The concentration of oxygen vacancies exhibited a maximum for Bi_(0.12)Ce_(0.88)O_(δ),which afforded the highest DMC production rate.Long-term tests showed stable activity and selectivity of this catalyst over 45 h on-stream at 140°C and a gas-hourly space velocity of 2,880 mL·g_(cat)^(-1)·h^(-1).In-situ modulation excitation diffuse reflection Fourier transform infrared spectroscopy and first-principle calculations indicate that the DMC synthesis occurs through reaction of a bidentate carbonate intermediate with the activated methoxy(-OCH_(3))species.The activation of C0_(2) to form the bidentate carbonate intermediate on the oxygen vacancy sites is identified as highest energy barrier in the reaction pathway and thus is likely the rate-determining step. | Yongdong Chen Yue Li Wei Chen Wen Wu Xu Zhong-kang Han Ammara Waheed Zhongbin Ye Gao Li Alfons Baiker | 2022 | Nano Research2022，15，2： | 2 |
| 3 | Selective Oxidation Catalysis: Opportunities and Challenges显示文摘 | Ive Hermans Eyal S. Spier Ulrich Neuenschwander Natascia Turrà Alfons Baiker | 2009 | Topics in Catalysis2009，，9： | 1 |
| 4 | Influence of grain morphology of V2O5 on its reducibility and selectivity for methanol oxidation显示文摘 | BAIKER A MONTI D | 1985 | J Catal1985，91，： | 1 |
| 5 | Preparation and structural properties of ultrafine gold colloids for oxidation catalysis显示文摘 | Duff D G Baiker A | 1995 | Studies in Surface Science and Catalysis1995，91，： | 1 |
| 6 | Reduction of nitrogen oxides over unsupported iridium: effect of reducing agent显示文摘 | W''ogerbauer C Maciejewski M Baiker A | 2001 | Applied Catalysis B: Environmental2001，34，： | 1 |
| 7 | Supercritical fluids in heterogeneous catalysis 显示文摘 | BAIKER A | 1999 | Chem Rev1999，99，2： | 1 |
| 8 | 显示文摘 | Marti P E Maeiejewski M Baiker A | 1994 | Applied Catalysis B: Environmental1994，4，23： | 1 |
| 9 | 查看详情显示文摘 | Thomas D J Wlli R Baiker A | | 0，，： | 1 |
| 10 | Supercritical CO2/ionic liquid systems? what can we extract from infrared andRaman spectra?显示文摘 | ANDANSON J M JUTZ F BAIKER A | 2009 | The Journal of Physical Chemistry B2009，113，10： | 1 |
| 11 | Silica hybrid gel catalysts containing ruthenium complexes: influence of reaction parameters on the catalytic behaviour in the synthesis of N, N-dimethylformamide from carbon dioxide显示文摘 | Krocher O Koppel R A Baiker A | 1999 | J Mol Catal A1999，140，2： | 1 |
| 12 | Investigation ofbinary and ternary systems of ionic liquids with water and/orsupercritical CO2 by in situ attenuated total reflection infraredspectroscopy显示文摘 | ANDANSON J M JUTZ F BAIKER A | 2010 | The Journal of Physical Chemistry B2010，114，6： | 1 |
| 13 | A mesoporous ruthenium silica hybrid aerogel with outstanding catalytic properties in the synthesis of N, N-diethylformamide from CO2,H2 and diethylamine 显示文摘 | Schmid L Rohr M Baiker A | 1999 | Chem Commun1999，22，： | 1 |
| 14 | NOx storage-reduction catalysis: From mechanism and materials properties to storage- reduction performance显示文摘 | Roy S Baiker A | 2009 | Chemical Reviews2009，109，9： | 1 |
| 15 | 查看详情显示文摘 | Rytz D W Baiker A | | 0，，： | 1 |
| 16 | 显示文摘 | | 1997 | J Mol Catal A:Chem1997，115，3： | 1 |
| 17 | Preparation of supported gold catalysts for low-temperature CO oxidation via 'size-controlled' gold colloids 显示文摘 | Grunwaldt J D Kiener C WSgerbauer C Baiker Alfons | 1999 | Journal of Catalysis1999，181，： | 1 |
| 18 | Quantitative calibration of spectroscopic signals in combined TG-FTIR system显示文摘 | EIGENMANN F MACIEJEWSKI M BAIKER A | 2006 | Thermochimica Acta2006，440，1： | 1 |
| 19 | Oxidation of alcohols with molecular oxygen on solid catalysts显示文摘 | MALLAT T BAIKER A | | 0，，06： | 1 |
| 20 | Autonomous navigation and map building using laser range sensors in outdoor applications显示文摘 | J Guivant E Nebot S Baiker | 2000 | Journal of Robotic Systems2000，17，10： | 1 |
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