Ni, Ru掺杂CePO4纳米材料的合成与仿酶性质

doi:10.7503/cjcu20200119

高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (5): 947.doi: 10.7503/cjcu20200119

• 庆祝《高等学校化学学报》复刊40周年专栏 • 上一篇下一篇

Ni, Ru掺杂CePO₄纳米材料的合成与仿酶性质

王启舜^1,²,张泽树¹,王欢¹,刘宇¹,宋术岩^1,^2,^*(),张洪杰^1,^2,^*()

^1. 中国科学院长春应用化学研究所, 稀土资源利用国家重点实验室, 长春 130022
^2. 中国科学技术大学应用化学与工程学院, 合肥 230026

收稿日期:2020-03-04 出版日期:2020-05-10 发布日期:2020-03-30
通讯作者: 宋术岩,张洪杰 E-mail:songsy@ciac.ac.cn;hongjie@ciac.ac.cn
基金资助:
国家自然科学基金(21590794);国家自然科学基金(21771173);中国科学院-澳大利亚联邦科工组织合作项目(GJHZ1730)

Synthesis and Enzymatic Activity of Ni, Ru Co-doped CePO₄ Nanomaterials ^†

WANG Qishun^1,²,ZHANG Zeshu¹,WANG Huan¹,LIU Yu¹,SONG Shuyan^1,^2,^*(),ZHANG Hongjie^1,^2,^*()

^1. State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences, Changchun 130022, China
^2. College of Applied Chemistry and Engineering,University of Science and Technology of China, Hefei 230026, China

Received:2020-03-04 Online:2020-05-10 Published:2020-03-30
Contact: Shuyan SONG,Hongjie ZHANG E-mail:songsy@ciac.ac.cn;hongjie@ciac.ac.cn
Supported by:
† Supported by the National Natural Science Foundation of China(21590794);† Supported by the National Natural Science Foundation of China(21771173);the Project of Chinese Academy of Sciences-Commonwealth Scientific and Industrial Research Organisation(CAS-CSIRO)(GJHZ1730)

摘要/Abstract

摘要：

通过水热方法合成了具有高比表面积的Ni, Ru掺杂CePO₄纳米粒子(NiRu-CePO₄). 结合纳米粒子的X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和X射线能谱(EDX)的表征结果发现, NiRu-CePO₄符合六方相磷酸铈, 纳米粒子长轴尺寸约为20 nm, Ni和Ru均匀分布于纳米CePO₄中; 样品的BET表面积高达178.4 m²/g, ζ电势为-18.2 mV. 以3,3',5,5'-四甲基联苯胺(TMB)作为电子供体和显色剂, 通过分光光度法监测652 nm处的吸光度值对产物浓度进行分析, 结果表明, NiRu-CePO₄催化剂在宽泛的pH范围内表现出类过氧化物酶和类氧化酶活性. 对催化后的催化剂进行表征, 发现样品形貌、元素分散性和表面Ce的价态均未显著变化, 表明NiRu-CePO₄具有较高的稳定性.

关键词: 磷酸铈, 钌, 双金属, 类过氧化物酶, 类氧化物酶

Abstract:

NiRu-CePO₄ nanoparticles with high specific surface area were synthesized by a simple hydrothermal method, which could avoid the separate nucleation process of the precious metal. The X-ray diffraction(XRD) pattern of NiRu-CePO₄ is consistent with hexagonal cerium phosphate. The transmission eletron microscopy(TEM) and energy dispersive X-ray(EDX) characterization indicated that the nanoparticles have a length of ca. 20 nm along the longitude and the doped metals Ni and Ru are uniformly dispersed. The BET area is determined as 178.4 m²/g, and the zeta potential as -18.2 mV. NiRu-CePO₄ exhibits good peroxidase-like and oxidase-like activities in wide pH range. 3,3',5,5'-tetramethylbenzidine(TMB) was used as the electron donor and the chromogenic reagent, and the activities were evaluated by monitoring the absorbance at 652 nm. The morphology, dispersion of the elements and valence state of Ce had no significant change when characterizing the used catalyst, confirming the good stability of NiRu-CePO₄.

Key words: Cerium phosphate, Ruthenium, Bimetal, Peroxidase mimic, Oxidase mimic

中图分类号:

O614

TrendMD:

王启舜, 张泽树, 王欢, 刘宇, 宋术岩, 张洪杰. Ni, Ru掺杂CePO₄纳米材料的合成与仿酶性质. 高等学校化学学报, 2020, 41(5): 947.

WANG Qishun, ZHANG Zeshu, WANG Huan, LIU Yu, SONG Shuyan, ZHANG Hongjie. Synthesis and Enzymatic Activity of Ni, Ru Co-doped CePO₄ Nanomaterials ^†. Chem. J. Chinese Universities, 2020, 41(5): 947.

图/表 7

Scheme 1 Synthetic procedure of NiRu-CePO4 (A) Direct synthesis; (B) hydroxide-assisted synthesis.

Fig.1 XRD pattern of NiRu-CePO4

Fig.2 SEM(A), TEM(B), HRTEM(C) and STEM-HAADF(D) images of NiRu-CePO4

Fig.3 STEM-HAADF image(A) and EDX mapping images of O(B), P(C), Ce(D), Ru(E) and Ni(F) of NiRu-CePO4

Fig.4 Time-course measurements(A), activities(B), pH(C) and temperature-depended(D) measurements of peroxidase-like activity of NiRu-CePO4 Time-course measurements were carried out with NiRu-CePO4 with various concentration under room temperature(ca. 20 ℃). Temperature-depended and pH-depended measurements were carried out with 200 μg/mL NiRu-CePO4.

Fig.5 XPS survey spectra(A) and high-resolution spectra of Ce3d(B) of NiRu-CePO4(a) and NiRu-CePO4 after peroxidase-like test(b)

Fig.6 Time-course measurements(A) and activities(B) of oxidase-like activity of NiRu-CePO4 Experiments were carried out with NiRu-CePO4 under room temperature(ca. 20 ℃) in pH=4 PBS buffer(25 mmol/L). The final concentrations of TMB were 1 mmol/L with various NiRu-CePO4 concentration.

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Ni, Ru掺杂CePO₄纳米材料的合成与仿酶性质

Synthesis and Enzymatic Activity of Ni, Ru Co-doped CePO₄ Nanomaterials ^†

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