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科研进展
李虎博士在国际学术期刊Applied Catalysis B和Green Chemistry发表学术论文
发布时间 : 2017-09-26   已浏览:

 高效低温从糖和羰基化物一步直接合成呋喃液体燃料

最近,国际学术期刊AppliedCatalysis B: Environmental(影响因子9.4,第一署名单位为南京农业大学,第一作者为博士后李虎,通讯作者为方真教授)及Green Chemistry【影响因子9.1,第一作者为李虎博士,通讯作者为杨松教授(贵州大学),Saravanamurugan博士(印度)和方真教授】,发表了生物燃料最新研究成果。

Efficient production offuranic/aromatic hydrocarbons (>95% yields) from biomass derivatives isachieved via a single-step process under mild conditions (25-130 ºC) by usingreadily available polymethylhydrosiloxane as liquid H-donor over hydrophonic Pdnanoparticles on MOFs.【以聚甲基氢硅氧烷为氢源,在低温条件下(25-130 ºC),利用疏水纳米钯Pd催化糖类(羰基和羟基化物),一锅高效(> 95%产量)合成呋喃液体燃料】

该研究团队开发了一个单步催化过程,以聚甲基氢硅氧烷polymethylhydrosiloxane(PMHS)为氢源,在低温条件下(25-130ºC),利用疏水纳米钯(Pd)催化糖类(羰基和羟基化物),单步高效(> 95%产量)合成呋喃液体燃料。

他们发现PMHS(带负电荷的高分子氢化物),作为绿色氢源,以纳米钯为催化剂,在原位加氢糖类合成呋喃醛/醇时,不会阻碍其上游的反应(例如,水解,异构化和脱水)。通过同位素氘标记研究证明,该反应系统可以一锅法,有选择地促进羰基和羟基化物的加氢脱氧。更重要的是,未还原的Pd(II)纳米催化剂在选择性加氢脱氧反应中也表现出相当的性能。此外,当该催化反应系统扩展到利用各种羰基化物时,可在室温下,定量生产相应的呋喃/芳烃。用聚二甲基硅氧烷涂层的疏水Pd催化剂具有极高的稳定性,且在至少连续五个周期中几乎没有失活和Pd浸出。

详情可见:

HLi, W Zhao,Zhen Fang*, Hydrophobic Pd Nanocatalysts for One-Pot andHigh-Yield Production of Liquid Furanic Biofuels at Low Temperatures,Applied Catalysis B: Environmental,215,18–27 (2017).

HLi, W Zhao, A Riisager, S Saravanamurugan*, Z Wang,Zhen Fang*, S Yang*,Pd-catalyzed in-situ domino process for mild andquantitative production of 2,5-dimethylfuran directly from carbohydrates, Green Chemistry,19, 2101–2106 (2017).

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Hydrophobic Pdnanocatalysts for one-pot and high-yield production of liquid furanic biofuelsat low temperatures    

Recently, Dr. Hu Li supervised by Prof. Zhen FANG has developeda single-step catalytic process for direct conversion of various saccharides toproduce furanic biofuels such as 2,5-dimethylfuran and 2-methylfuran with highyields (> 95%) at 110-130 ºC. The negatively charged hydride (H-) of readilyavailable polymethylhydrosiloxane (PMHS) acting as green H-donor overhydrophobic Pd nanoparticles did not obstruct upstream reactions (e.g.,hydrolysis, isomerization and dehydration) for the in situ formation of furanicaldehydes/alcohols from sugars, and could selectively facilitate the subsequenthydrodeoxygenation of carbonyl and hydroxyl groups other than the furanic ringin one pot, as clarified by deuterium-labeling study. Importantly, theunreduced Pd(II) catalysts also exhibited comparable performance in theselective hydrodeoxygenation reaction. Moreover, the catalytic strategy wasextended to various carboxides for quantitative production of correspondingfuranic/aromatic hydrocarbons at room temperature that were more pronouncedthan previously reported results, and the optimal Pd/MIL-53(Al) coated withpolydimethylsiloxane (Pd/MIL-53(Al)-P) was highly stable with littledeactivation and Pd leaching for at least five consecutive cycles.

Relatedresults were published:

HLi, W Zhao,Zhen Fang*, Hydrophobic Pd Nanocatalysts for One-Pot andHigh-Yield Production of Liquid Furanic Biofuels at Low Temperatures,Applied Catalysis B: Environmental,215,18–27 (2017).

HLi, W Zhao, A Riisager, S Saravanamurugan*, Z Wang,Zhen Fang*, S Yang*,Pd-catalyzed in-situ domino process for mild andquantitative production of 2,5-dimethylfuran directly from carbohydrates, Green Chemistry,19, 2101–2106 (2017).

上一条:杨守峰、仲高艳科研团队在Ceramics International上发表论文,阐述聚醚醚酮/羟基磷灰石(PEEK/HA)复合材料3D打印构建骨生物工程支架独特方法 下一条:方真教授获2017年度中国科学院优秀导师奖

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