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| 论文编号: |
122214O120130099 |
| 第一作者所在部门: |
902组 |
| 中文论文题目: |
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| 英文论文题目: |
An Introduction of CO2 Conversion by Dry Reforming with Methane and New Route of Low-Temperature Methanol Synthesis
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| 论文题目英文: |
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| 作者: |
椿范立
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| 论文出处: |
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| 刊物名称: |
ACCOUNTS OF CHEMICAL RESEARCH
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| 年: |
2013
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| 卷: |
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| 期: |
1 |
| 页: |
xx-xx |
| 联系作者: |
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| 收录类别: |
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| 影响因子: |
20.833
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| 摘要: |
Carbon dioxide is one of the highest contributors to the greenhouse effect, as well as a cheap and nontoxic building block for single carbon source chemistry. As such, CO2 conversion is one of most important research areas in energy and environment sciences, as well as in catalysis technology. For chem-ical conversion of CO2, natural gas (mainly CH4) is a promising counterpart molecule to the CO2-related reaction, due to its high availability and low price.More importantly, being able to convert CH4 to useful fuels and molecules is advantageous, because it is also a kind of“ greenhouse effect ” gas, and can be an energy alternative to petroleum oil. In this Account, we discuss our development of efficient catalysts with precisely designed nanostructure for CO2 reforming of CH4 to produce syngas (mixture of CO and H2
), which can then be converted to many chemicals and energy products. This new production flow can establish a GTL (gas-to-liquid) industry, being currently pushed by the shale gas revolution.From the viewpoint of GTL industry, developing a catalyst for CO2 reforming of CH4 is a challenge, because they need a very high production rate to make the huge GTL methane reformer as small as possible. In addition, since both CO2 and CH4 give off carbon deposits that deactivate non-precious metallic catalysts very quickly, the total design of catalyst support and supported metallic nanoparticles is necessary. We present a simple but useful method to prepare bimodal catalyst support, where small pores are formed inside large ones during the self-organization of nanoparticles from solution. Large pores enhance the mass
transfer rate, while small pores provide large surface areas to disperse active metallic nanoparticles. More importantly, building materials for small pores can also be used as promoters or cocatalysts to further enhance the total activity and stability.Produced syngas from methane reforming is generally catalytically converted in situ via one of two main routes. The first is to use Fischer Tropsch synthesis (FTS), a process that catalytically converts syngas to hydrocarbons of varying molecular weights.The second is methanol synthesis. The latter has better atomic economy, since the oxygen atom in CO is included in the product and CO2 can b e b lended into syngas a s a reactant. However, production of methanol is very inefficient i n this reaction: only 10 15% one-pass conversion typically a t 5 .0 10.0 MPa and 523 573 K, due to t he severe thermodynamic lim itations of this exothermal reaction(CO+2H2=CH3OH) . In this Account, w e pro pose and develop a n ew rout e o f low-temperature methanol synt hesis from CO2-containing syngas only b y a dding alcohols, including methanol itself. These alcohols act as homogeneous cocatalysts and the solvent, realizing 70-100% one-pass conversion at only 5.0 MPa and 443 K. The key step i s t he reaction of the a dsorbed formate species w ith a lcohols to yield e ster species at l ow temperatures, f ollowed by the hydr ogenation of ester by hydrogen a toms on metallic Cu. This changes t he
normal reaction path o f conventional, high-temperature methanol synthesis from formate via m ethoxy to methanol. |
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