Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh-Pd/C Catalysts

doi:10.1021/acsami.4c06180

	Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh-Pd/C Catalysts
	Gong, Xutao 1,2; Qin, Shuting 2; Li, Tong 1,2; Wei, Xinghua 2; Liu, Sujing 2; Liu, Ying 2; Ma, Xuanxuan 2; Li, Qing3 ; Xia, Chuanhai1,2
发表期刊	ACS APPLIED MATERIALS & INTERFACES
ISSN	1944-8244
	2024-08-08
卷号	16 期号:33 页码:43474-43488
关键词	4-fluorophenol synergisticeffect hydro-defluorination(HDF) Pd-Rh/C reducing agent
DOI	10.1021/acsami.4c06180
通讯作者	Ma, Xuanxuan([email protected]) ; Xia, Chuanhai([email protected])
英文摘要	This study explores the synergistic effect between the Rh and Pd of bimetallic Rh-Pd/C catalysts for the catalytic hydro-defluorination (HDF) of 4-fluorophenol (4-FP). It was found that 4-FP could not be efficiently hydro-defluorinated over 6% Pd/C and 6% Rh/C due to the inherent properties of Pd and Rh species in the dissociation of H-2 and the activation of C-F bonds. Compared with 6% Pd/C and 6% Rh/C, bimetallic Rh-Pd/C catalysts, especially 1% Rh-5% Pd/C, exhibited much higher catalytic activity in the HDF of 4-FP, suggesting that the synergistic effect between the Rh and Pd of the catalyst was much more positive. Catalyst characterizations (BET, XRD, TEM, and XPS) were introduced to clarify the mechanism for the synergistic effect between the Rh and Pd of the catalyst in the HDF reaction and revealed that it was mainly attributed to the bifunctional mechanism: Pd species were favorable for the dissociation of H-2, and Rh species were beneficial to the activation of C-F bonds in the HDF reaction. Meanwhile, the interaction between Rh and Pd species enabled Rh and Pd to exhibit a more positive synergistic effect, which promoted the migration of atomic H* from Pd to Rh species and thus enhanced the HDF of 4-FP. Furthermore, 1% Rh-5% Pd/C prepared using 20-40 equiv NaBH4 exhibited the best performance in the catalytic HDF of 4-FP. Catalysis characterizations suggested that appropriate Rh3+/Rh-0 and Pd2+/Pd-0 ratios were beneficial to the dissociation of H-2 and the activation of C-F bonds, which caused the more positive synergistic effect between the Rh and Pd of Rh-Pd/C in the HDF reaction. This work offers a valuable strategy for enhancing the performance of catalytic HDF catalysts via promoting synergistic effects.
资助机构	Youth Innovation Technology Project of Higher School in Shandong Province ; National Natural Science Foundation of China ; Natural Science Foundation of Shandong Province of China
收录类别	SCI
语种	英语
关键词[WOS]	LIQUID-PHASE HYDRODECHLORINATION ; ELECTROCHEMICAL HYDRODEFLUORINATION ; WATER ; HYDROGENATION ; OXIDATION ; KINETICS ; ATOM
研究领域[WOS]	Science & Technology - Other Topics ; Materials Science
WOS记录号	WOS:001287549500001
引用统计
文献类型	期刊论文
条目标识符	http://ir.yic.ac.cn/handle/133337/35838
专题	海岸带生物学与生物资源利用重点实验室海岸带生物学与生物资源利用重点实验室_海岸带生物资源高效利用研究与发展中心
通讯作者	Ma, Xuanxuan; Xia, Chuanhai
作者单位	1.Ludong Univ, Inst Adv Study Coastal Ecol, Yantai 264025, Peoples R China 2.Ludong Univ, Sch Resources & Environm Engn, Yantai 264025, Peoples R China 3.Chinese Acad Sci, Yantai Inst Coastal Zone Res, Key Lab Coastal Biol & Bioresource Utilizat, Yantai 264003, Peoples R China
推荐引用方式 GB/T 7714	Gong, Xutao,Qin, Shuting,Li, Tong,et al. Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh-Pd/C Catalysts[J]. ACS APPLIED MATERIALS & INTERFACES,2024,16(33):43474-43488.
APA	Gong, Xutao.,Qin, Shuting.,Li, Tong.,Wei, Xinghua.,Liu, Sujing.,...&Xia, Chuanhai.(2024).Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh-Pd/C Catalysts.ACS APPLIED MATERIALS & INTERFACES,16(33),43474-43488.
MLA	Gong, Xutao,et al."Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh-Pd/C Catalysts".ACS APPLIED MATERIALS & INTERFACES 16.33(2024):43474-43488.