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Direct Amination of Biomass‐based Furfuryl Alcohol and 5‐(Aminomethyl)‐2‐furanmethanol with NH3 over Hydrotalcite‐derived Nickel Catalysts via the Hydrogen‐borrowing Strategy
ChemCatChem ( IF 3.8 ) Pub Date : 2021-02-23 , DOI: 10.1002/cctc.202001922 Kuo Zhou 1, 2 , Ruihong Xie 1 , Meiting Xiao 1 , Darun Guo 1 , Zhuodi Cai 1 , Shimin Kang 1 , Yongjun Xu 1 , Jinjia Wei 2
ChemCatChem ( IF 3.8 ) Pub Date : 2021-02-23 , DOI: 10.1002/cctc.202001922 Kuo Zhou 1, 2 , Ruihong Xie 1 , Meiting Xiao 1 , Darun Guo 1 , Zhuodi Cai 1 , Shimin Kang 1 , Yongjun Xu 1 , Jinjia Wei 2
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A series of hydrotalcite‐derived nickel catalysts were synthesized and employed for the direct amination of biomass‐based furfuryl alcohol with NH3 via the hydrogen borrowing strategy. The effects of the Ni/Al molar ratio and calcination temperature of the NiAl hydrotalcite‐like precursors on the performance of the NixAl‐CT catalyst were investigated. The systematic characterization showed that the synergistic catalysis of the metal and acid‐base sites was of vital importance for the amination of alcohols. In particular, the Ni2Al‐600 catalyst with high amount of Ni0 sites (1.26 mmol g−1) and suitable density of acid‐base sites (0.71 mmol g−1 and 1.10 mmol g−1, respectively) exhibited the best dehydrogenation capability and therefore excellent catalytic activity. An 84.1 % yield of furfurylamine with complete conversion of furfuryl alcohol was obtained under the reaction conditions of 180 °C and 0.4 MPa NH3 in 36 h. The presence of Ni3N in the spent catalyst, confirmed by XRD, TEM and XPS characterizations, was demonstrated to be responsible for the deactivation of the NixAl‐CT catalyst. In addition, the Ni2Al‐600 catalyst exhibited satisfactory performance toward another important biomass‐related transformation of 5‐(aminomethyl)‐2‐furanmethanol to 2,5‐bis(aminomethyl)furan, with a yield of 70.5 %.
中文翻译：
通过水借方策略在水滑石衍生的镍催化剂上用NH3直接氨化生物质糠醇和5-（氨基甲基）-2-呋喃甲醇
合成了一系列水滑石衍生的镍催化剂，并通过氢借用策略将其用于用NH 3与基于生物质的糠醇直接胺化。研究了Ni / Al摩尔比和NiAl类水滑石前体的煅烧温度对Ni x Al-CT催化剂性能的影响。系统表征表明，金属和酸碱位的协同催化对于醇的胺化至关重要。特别是具有大量Ni 0位（1.26 mmol g -1）和合适的酸碱位密度（0.71 mmol g -1和1.10 mmol g -1）的Ni 2 Al-600催化剂分别显示出最佳的脱氢能力，因此具有出色的催化活性。在180°C和0.4 MPa NH 3的反应条件下，在36小时内，糠醇完全转化的糠胺产率为84.1％。XRD，TEM和XPS表征证实了废催化剂中Ni 3 N的存在是Ni x Al-CT催化剂失活的原因。此外，Ni 2 Al-600催化剂对另一重要的生物量相关的5-（氨基甲基）-2-呋喃甲醇向2,5-双（氨基甲基）呋喃的转化表现出令人满意的性能，产率为70.5％。
更新日期：2021-04-22
中文翻译：
通过水借方策略在水滑石衍生的镍催化剂上用NH3直接氨化生物质糠醇和5-（氨基甲基）-2-呋喃甲醇
合成了一系列水滑石衍生的镍催化剂，并通过氢借用策略将其用于用NH 3与基于生物质的糠醇直接胺化。研究了Ni / Al摩尔比和NiAl类水滑石前体的煅烧温度对Ni x Al-CT催化剂性能的影响。系统表征表明，金属和酸碱位的协同催化对于醇的胺化至关重要。特别是具有大量Ni 0位（1.26 mmol g -1）和合适的酸碱位密度（0.71 mmol g -1和1.10 mmol g -1）的Ni 2 Al-600催化剂分别显示出最佳的脱氢能力，因此具有出色的催化活性。在180°C和0.4 MPa NH 3的反应条件下，在36小时内，糠醇完全转化的糠胺产率为84.1％。XRD，TEM和XPS表征证实了废催化剂中Ni 3 N的存在是Ni x Al-CT催化剂失活的原因。此外，Ni 2 Al-600催化剂对另一重要的生物量相关的5-（氨基甲基）-2-呋喃甲醇向2,5-双（氨基甲基）呋喃的转化表现出令人满意的性能，产率为70.5％。
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