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Synergistic catalysis of Pd single atoms and Pd nanoparticles for cinnamaldehyde hydrogenation to phenylpropanal
- Low-carbon Chemistry and Chemical Engineering Vol. 50, Issue 2, Pages: 45-52(2025)
- 作者机构：
1.大连交通大学 环境与化学工程学院，辽宁 大连 116028
2.中国科学院 大连化学物理研究所，辽宁 大连 116023
3.西南石油大学 化学化工学院，四川 成都 610500
4.四川大学 化学工程学院，四川 成都 610065
- 作者简介：
- 基金信息：
DOI：10.12434/j.issn.2097-2547.20240223
CLC： TQ426;O643.3Received：21 May 2024，
Revised：11 June 2024，
Published：25 February 2025
- 稿件说明：
移动端阅览
任小敏,赵芋衡,马颖等.Pd单原子和Pd纳米颗粒协同催化肉桂醛加氢制苯丙醛[J].低碳化学与化工,2025,50(02):45-52.
REN Xiaomin,ZHAO Yuheng,MA Ying,et al.Synergistic catalysis of Pd single atoms and Pd nanoparticles for cinnamaldehyde hydrogenation to phenylpropanal[J].Low-carbon Chemistry and Chemical Engineering,2025,50(02):45-52.
任小敏,赵芋衡,马颖等.Pd单原子和Pd纳米颗粒协同催化肉桂醛加氢制苯丙醛[J].低碳化学与化工,2025,50(02):45-52. DOI： 10.12434/j.issn.2097-2547.20240223.
REN Xiaomin,ZHAO Yuheng,MA Ying,et al.Synergistic catalysis of Pd single atoms and Pd nanoparticles for cinnamaldehyde hydrogenation to phenylpropanal[J].Low-carbon Chemistry and Chemical Engineering,2025,50(02):45-52. DOI： 10.12434/j.issn.2097-2547.20240223.
摘要
由于肉桂醛（CAL）分子中的两个不饱和化学键构成了复杂的共轭体系，CAL分子中的C==C和C==O键进行选择性加氢以生成所需产物是一项具有挑战性的工作。分别制备了Pd单原子、Pd纳米颗粒及Pd单原子和纳米颗粒共同负载在纳米金刚石（ND）的催化剂（分别为Pd
1
/ND（
w
(Pd) = 0.05%）、Pd
NPs
/ND（
w
(Pd) = 0.25%）和Pd
1+NPs
/ND（
w
(Pd) = 0.25%）），并研究了Pd的几何和电子结构对催化剂催化CAL加氢性能的影响。通过HR-TEM、XRD和XPS等方法对ND进行了表征。结果表明，ND是一种表面含有丰富氧官能团且具有单原子锚定位点的高结晶度及高表面能的载体。同时利用HADDF-STEM、AC-TEM和XPS等方法对Pd
1+NPs
/ND的几何和电子结构进行了分析。结果表明，与Pd/C相比，Pd
1+NPs
/ND具有更高的
n
(Pd
δ
+
)/
n
(Pd
0
)，进一步证实了Pd
1+NPs
/ND上Pd单原子和Pd颗粒共存。在反应温度为40 ℃、H
2
压力为1 MPa和
n
(Pd)/
n
(CAL)为0.023%的条件下，分别考察了Pd
1+NPs
/ND、Pd/C、Pd
1
/ND和Pd
NPs
/ND对CAL加氢反应的催化性能。结果表明，Pd
1+NPs
/ND表现出远高于Pd/C的催化活性和苯丙醛（HCAL）选择性，Pd
1
/ND和Pd
NPs
/ND均表现出较低的催化活性。因此，在Pd
1+NPs
/ND高效催化CAL加氢反应中，Pd单原子和Pd纳米颗粒之间存在协同效应。
Abstract
Due to the complex conjugated structure of the two unsaturated chemical bonds in cinnamaldehyde (CAL) molecules
the selective hydrogenation of C==C and C==O bonds in CAL to produce desired products is a chal
lenging task. Pd single atoms
Pd nanoparticles and a combination of Pd single atoms and Pd nanoparticles supported on nanodiamonds (ND) were prepared (Pd
1
/ND（
w
(Pd) = 0.05%）
Pd
NPs
/ND（
w
(Pd) = 0.25%）and Pd
1+NPs
/ND（
w
(Pd) = 0.25%）
respectively). The influences of the geometric and electronic structures of Pd on catalytic performances of catalysts in CAL hydrogenation were studied. The ND was characterized by HR-TEM
XRD and XPS. The results show that ND is a kind of high-crystallinity and high-surface-energy support with abundant oxygen functional groups and single-atom anchoring sites. The geometric and electronic structures of Pd
1+NPs
/ND were analyzed by HADDF-STEM
AC-TEM and XPS. The results show that compared to Pd/C
Pd
1+NPs
/ND has higher
n
(Pd
δ
+
)/
n
(Pd
0
)
further confirming the coexistence of Pd single atoms and Pd nanoparticles. The catalytic performances of Pd
1+NPs
/ND
Pd/C
Pd
1
/ND and Pd
NPs
/ND for CAL hydrogenation were investigated under the conditions of the temperature of 40 ℃
the H
2
pressure of 1 MPa and
n
(Pd)/
n
(CAL) of 0.023%. The results show that Pd
1+NPs
/ND exhibites much higher catalytic activity and hydrocinnamaldehyde (HCAL) selectivity than Pd/C. Pd
1
/ND and Pd
NPs
/ND show low catalytic activities. Therefore
there is a synergistic effect between Pd single atoms and Pd nanoparticles in the efficient catalytic CAL hydrogenation by Pd
1+NPs
/ND.
关键词
Keywords
references
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