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| 1 | PdCo/SiO_(2)双金属催化剂用于杂环储氢载体的高效脱氢显示文摘乙基咔唑/十二氢乙基咔唑(N-ethylcarbazole/dodecahydro-N-ethylcarbazole,NECZ/12H-NECZ)体系被认为在有机液体储氢领域具有较大的开发应用前景,但高活性、选择性的脱氢催化剂的设计开发制约着其工业应用。基于此,设计开发出一种具有高脱氢活性和高选择性的双金属催化剂Pd_(1)Co_(3)/SiO_(2)(Pd质量分数为1.25%),对其结构进行了XPS、XRD、HRTEM等表征分析,并评价了其催化十二氢乙基咔唑的脱氢性能。与5.0%(质量分数)Pd/SiO_(2)相比,表明引入一定量的Co金属形成的PdCo合金可提高12H-NECZ脱氢反应效率和NECZ选择性,动力学与DFT计算发现双金属催化剂可以有效降低三步基元反应的能垒,大幅提升第二步基元反应(8H-NECZ到4H-NECZ)的脱氢反应速率。研究结果为揭示12H-NECZ脱氢反应机理和高效脱氢反应催化剂的设计与开发提供了新的思路。 | 龚翔 李林森 姜召 | 2022 | 化工学报2022，73，10： | 0 |
| 2 | Recent advances in Raman spectroelectrochemistry on single-crystal surfaces显示文摘Benefiting from a principally contaminant-free and well-defined surface,single-crystal electrodes offer new insights into interfacial processes and are important in electrochemistry.The early impetus for using single-crystal electrodes in electrocatalysis was to investigate the surface structure at the atomic level for the reactions that are sensitive to the surface.These studies were usually performed in an ultra-high vacuum with atomic force microscopy(AFM),scanning tunneling microscope(STM),and X-ray methods to avoid the contamination.However,such characterizations are limited in their ability to identify chemical species definitively,a limitation that has similarly plagued the study of single-crystals.Recent advances in shellisolated nanoparticle-enhanced Raman spectroscopy(SHINERS)have enabled the detection of reaction intermediates on singlecrystal electrodes,in which shell-isolated nanoparticles on the single-crystal electrode can enhance the Raman signal from the surface,without changing the surface structure and electrochemical response.Thus,this work aims to review recent advances in Raman spectroelectrochemical studies on single-crystal electrode surfaces.The discussion focuses on how SHINERS technology has enabled the effective detection of intermediate species and,when combined with the electrochemical method,has yielded novel insights into the dynamic evolution of surface structure and electrocatalytic reaction mechanisms.Finally,the challenges and future of single-crystal electrodes are introduced. | Quan-Feng He Jia Yu Jin-Chao Dong Jian-Feng Li | 2023 | Science China Chemistry2023，66，12： | 0 |
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