低碳化学与化工2025，Vol.50Issue(2)：45-52,8.DOI:10.12434/j.issn.2097-2547.20240223
Pd单原子和Pd纳米颗粒协同催化肉桂醛加氢制苯丙醛
Synergistic catalysis of Pd single atoms and Pd nanoparticles for cinnamaldehyde hydrogenation to phenylpropanal
摘要
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 challenging task.Pd single atoms,Pd nanoparticles and a combination of Pd single atoms and Pd nanoparticles supported on nanodiamonds(ND)were prepared(Pd1/ND(w(Pd)=0.05%),PdNPs/ND(w(Pd)=0.25%)and Pd1+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 Pd1+NPs/ND were analyzed by HADDF-STEM,AC-TEM and XPS.The results show that compared to Pd/C,Pd1+NPs/ND has higher n(Pdδ+)/n(Pd0),further confirming the coexistence of Pd single atoms and Pd nanoparticles.The catalytic performances of Pd1+NPs/ND,Pd/C,Pd1/ND and PdNPs/ND for CAL hydrogenation were investigated under the conditions of the temperature of 40℃,the H2 pressure of 1 MPa and n(Pd)/n(CAL)of 0.023%.The results show that Pd1+NPs/ND exhibites much higher catalytic activity and hydrocinnamaldehyde(HCAL)selectivity than Pd/C.Pd1/ND and PdNPs/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 Pd1+NPs/ND.关键词
Pd单原子/Pd纳米颗粒/纳米金刚石/肉桂醛加氢/协同催化Key words
Pd single atoms/Pd nanoparticles/nanodiamond/cinnamaldehyde hydrogenation/synergetic catalysis分类
化学化工引用本文复制引用
任小敏,赵芋衡,马颖,张啟霞,马军,刘岳峰..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(2):45-52,8.基金项目
国家自然科学基金(22172161,22302027) （22172161,22302027）
大连市青年科技之星项目(2022RQ030) （2022RQ030）
榆林中科洁净能源创新研究院人工智能科技专项(DNL-YLA202204). （DNL-YLA202204）
