Pt3Co高指数晶面氧还原过程的密度泛函理论研究

doi:10.15541/jim20240296

无机材料学报 ›› 2025, Vol. 40 ›› Issue (1): 39-46.DOI: 10.15541/jim20240296 CSTR: 32189.14.10.15541/jim20240296

Pt₃Co高指数晶面氧还原过程的密度泛函理论研究

刘磊¹^,²^,³(), 郭瑞华¹^,²^,³(), 王丽⁴, 王艳⁵, 张国芳¹, 关丽丽¹^,²

1.内蒙古科技大学材料科学与工程学院, 包头 014010
2.内蒙古科技大学内蒙古自治区先进陶瓷材料与器件重点实验室, 包头 014020
3.内蒙古科技大学轻稀土资源绿色提取与高效利用教育部重点实验室, 包头 014020
4.内蒙古科技大学化学与化工学院包头 014010
5.内蒙古科技大学包头稀土研究院包头 014020

收稿日期:2024-06-18 修回日期:2024-08-23 出版日期:2025-01-20 网络出版日期:2024-09-02
通讯作者: 郭瑞华, 教授. E-mail: grh7810@163.com
作者简介:刘磊(2000-), 男, 硕士研究生. E-mail: 1371281920@qq.com
基金资助:
国家自然科学基金(51864040);国家自然科学基金(51962028);国家自然科学基金(52162010);内蒙古自治区科技计划(2021GG0042);内蒙古自治区高等学校青年科技英才(NJYT22064);内蒙古自治区自然科学基金(2022MS05018);内蒙古自治区自然科学基金(2022LHMS05021)

Oxygen Reduction Reaction on Pt₃Co High-index Facets by Density Functional Theory

LIU Lei¹^,²^,³(), GUO Ruihua¹^,²^,³(), WANG Li⁴, WANG Yan⁵, ZHANG Guofang¹, GUAN Lili¹^,²

1. School of Materials Science and Engineering, Inner Mongolia University of Science & Technology, Baotou 014010, China
2. Inner Mongolia Key Laboratory of Advanced Ceramic Materials and Devices, Inner Mongolia University of Science & Technology, Baotou 014010, China
3. Key Laboratory of Green Extraction & Efficient Utilization of Light Rare-Earth Resources, Ministry of Education, Inner Mongolia University of Science & Technology, Baotou 014010, China
4. School of Chemistry and Chemical Engineering, Inner Mongolia University of Science & Technology, Baotou 014010, China
5. Baotou Research Institute of Rare Earths, Baotou 014020, China

Received:2024-06-18 Revised:2024-08-23 Published:2025-01-20 Online:2024-09-02
Contact: GUO Ruihua, professor. E-mail: grh7810@163.com
About author:LIU Lei (2000-), male, Master candidate. E-mail: 1371281920@qq.com
Supported by:
National Natural Science Foundation of China(51864040);National Natural Science Foundation of China(51962028);National Natural Science Foundation of China(52162010);Inner Mongolia Autonomous Region Science and Technology Program(2021GG0042);Inner Mongolia Autonomous Region Youth Science and Technology Excellence in Higher Education(NJYT22064);Inner Mongolia Autonomous Region Natural Science Foundation Program(2022MS05018);Inner Mongolia Autonomous Region Natural Science Foundation Program(2022LHMS05021)

摘要/Abstract

摘要：

Pt₃Co催化剂是Pt基合金中氧还原反应(ORR)活性最高的催化剂, 合成Pt₃Co高指数晶面(HIFs)是一种提高其催化性能的有效策略, 但拥有最高ORR活性的HIFs尚未明确, 并且目前缺乏对Pt₃Co HIFs ORR的系统研究。本研究构建了六种不同Pt₃Co HIFs, 通过从头算分子动力学(AIMD)计算证明了其稳定性, 通过密度泛函理论(DFT)计算了六种Pt₃Co HIFs的ORR过程中间物*O、*OH、*OOH的结合能(BE), 通过d带中心(ε_d)、Bader电荷及配位数(CN)解释了其在台阶与边缘位点BE不同的原因。同时分析了吸附原子CN与ε_d的关系, 通过ORR自由能台阶图分析了ORR过程中的过电位(η), 发现η大小主要与*OH结合能(BE-*OH)有关, 其中η最小的晶面为Pt₃Co(211), 其在台阶处的η达到了0.294 eV。本工作为高ORR活性HIFs催化剂研发提供了一定的理论依据。

关键词: Pt₃Co催化剂, 高指数晶面, 密度泛函理论, 氧还原反应

Abstract:

Pt₃Co catalyst is the most active catalyst for oxygen reduction reaction (ORR) in Pt based alloys, in which synthesis of Pt₃Co high-index facets (HIFs) is an effective strategy to improve its catalytic performance. However, HIFs possessing the highest ORR activity have not yet been clarified, and at present, there is a lack of a systematic study on the ORR of Pt₃Co HIFs. In this study, six different Pt₃Co HIFs were constructed, and their stability was proved through ab initio molecular dynamics (AIMD) calculations. Binding energies (BE) of *O, *OH and *OOH intermediates for the six Pt₃Co HIFs during ORR process were calculated by density functional theory (DFT), and d-band center (ε_d), Bader charge and coordination number (CN) were used to explain the different binding energies at terrace and edge sites. Relationship between CN of adsorbed atoms and ε_d was also analyzed. Overpotential (η) during ORR was analyzed through ORR free energy step diagram, and it revealed that the magnitude of η was mainly related to *OH binding energy (BE-*OH). The Pt₃Co(211) facet has the smallest η, which at the Pt₃Co(211) terrace site reaches 0.294 eV. Therefore, this work provides a sound theoretical basis for the development of high ORR activity HIFs catalysts.

Key words: Pt₃Co catalyst, high-index facet, density functional theory, oxygen reduction reaction

中图分类号:

TM911

刘磊, 郭瑞华, 王丽, 王艳, 张国芳, 关丽丽. Pt₃Co高指数晶面氧还原过程的密度泛函理论研究[J]. 无机材料学报, 2025, 40(1): 39-46.

LIU Lei, GUO Ruihua, WANG Li, WANG Yan, ZHANG Guofang, GUAN Lili. Oxygen Reduction Reaction on Pt₃Co High-index Facets by Density Functional Theory[J]. Journal of Inorganic Materials, 2025, 40(1): 39-46.

图/表 20

图1 不同HIFs表面原子结构模型的三角示意图

Fig. 1 Triangle diagram of surface atomic structure models with different HIFs

图2 Pt3Co原胞及六个Pt3Co HIFs的表面模型

Fig. 2 Surface models of Pt3Co unitcell and six Pt3Co HIFs (a) Pt3Co unitcell; (b) Pt3Co(211); (c) Pt3Co(310); (d) Pt3Co(331); (e) Pt3Co(511); (f) Pt3Co(320); (g) Pt3Co(332)

图3 (a)HIFs台阶和边缘位置示意图, 以及(b)*O、*OH、*OOH在Pt3Co(211)边缘处的最佳吸附构型

Fig. 3 (a) Schematic representation of HIFs terrace and edge positions, and (b) optimal adsorption configurations of *O, *OH, and *OOH at Pt3Co(211) edge

表1 不同反应中间物在六个HIFs不同位置的BE与BD

Table 1 BE and BD of different reaction intermediates at different positions of six Pt3Co HIFs

HIFs	Site	*O		*OH		*OOH
HIFs	Site	BE/eV	BD/nm	BE/eV	BD/nm	BE/eV	BD/nm
Pt₃Co(211)	Edge	3.043	0.195	0.903	0.213	3.643	0.217
Pt₃Co(211)	Terrace	2.334	0.206	0.936	0.200	3.658	0.206
Pt₃Co(310)	Edge	1.505	0.179	0.341	0.195	3.484	0.196
Pt₃Co(310)	Terrace	1.405	0.197	0.674	0.213	3.828	0.212
Pt₃Co(331)	Edge	1.175	0.194	0.620	0.214	3.499	0.216
Pt₃Co(331)	Terrace	1.512	0.208	0.838	0.200	3.702	0.221
Pt₃Co(511)	Edge	1.291	0.192	0.524	0.212	3.633	0.215
Pt₃Co(511)	Terrace	1.335	0.197	0.599	0.213	3.789	0.214
Pt₃Co(320)	Edge	1.204	0.179	0.105	0.195	3.218	0.193
Pt₃Co(320)	Terrace	1.638	0.181	0.356	0.197	3.473	0.199
Pt₃Co(332)	Edge	1.418	0.194	0.576	0.215	3.419	0.214
Pt₃Co(332)	Terrace	1.618	0.201	0.723	0.215	3.778	0.212

表2 六个Pt3Co HIFs不同位置Pt原子的Bader电荷转移数和εd

Table 2 Bader charge transfer number and εd of Pt atoms at different positions of six Pt3Co HIFs

HIFs	Pt₃Co(211)	Pt₃Co(310)	Pt₃Co(331)	Pt₃Co(511)	Pt₃Co(320)	Pt₃Co(332)
Bader charge transfer number (edge)/e	0.199	0.206	0.187	0.173	0.214	0.182
Bader charge transfer number (terrace)/e	0.185	0.149	0.194	0.138	0.170	0.203
ε_d (edge)/eV	-1.502	-1.560	-1.683	-1.746	-1.530	-1.671
ε_d (terrace)/eV	-1.729	-1.667	-1.820	-1.831	-1.707	-1.836

图4 (a)依据CN标识的表面台阶和边缘位置示意图, 以及(b)六个HIFs吸附原子εd和CN的关系

Fig. 4 (a) Schematic representation of the positions of surface terrace and edge identified on the basis of CN, and (b) relationships of εd and CN for the six HIFs adsorbed atoms Colorful figures are available on website

图5 Pt3Co HIFs催化剂在台阶处ORR自由能变化图

Fig. 5 Plots of ORR free energy at terrace for Pt3Co HIFs catalysts (a) Pt3Co(211); (b) Pt3Co(310); (c) Pt3Co(331); (d) Pt3Co(511); (e) Pt3Co(320); (f) Pt3Co(332)

图6 ηORR与BE-*OH的关系图

Fig. 6 Plots of ηORR and BE-*OH (a) Edge; (b) Terrace

表3 六个Pt3Co HIFs在不同位置的ηORR

Table 3 Bader charge transfer number and εd of Pt atoms at different positions of six Pt3Co HIFs

HIFs	Pt₃Co(211)	Pt₃Co(310)	Pt₃Co(331)	Pt₃Co(511)	Pt₃Co(320)	Pt₃Co(332)
η_ORR (edge)/eV	0.630	0.889	0.675	0.706	1.125	0.654
η_ORR (terrace)/eV	0.294	0.556	0.556	0.631	0.874	0.507

表S1 六个HIFs的微面标记方式、k点、原子数

Table S1 Microfact notation, k-point, number of atoms of six HIFs

HIFs	Microfact notation	k-point	Number of atoms
Pt₃Co(211)	n(111)×(100)	3×2×1	48
Pt₃Co(310)	n(100)×(110)	3×2×1	48
Pt₃Co(331)	n(110)×(111)	2×2×1	48
Pt₃Co(511)	n(100)×(111)	2×2×1	48
Pt₃Co(320)	n(110)×(100)	3×2×1	48
Pt₃Co(332)	n(111)×(110)	2×2×1	48

表S2 六个HIFs不同位置的BE-*OH与εd

Table S2 BE-*OH and εd at different positions of six HIFs

HIFs	Site	BE-*OH/eV	ε_d/eV
Pt₃Co(211)	Edge	0.903	-1.502
Pt₃Co(211)	Terrace	0.936	-1.729
Pt₃Co(310)	Edge	0.341	-1.746
Pt₃Co(310)	Terrace	0.674	-1.831
Pt₃Co(331)	Edge	0.620	-1.560
Pt₃Co(331)	Terrace	0.838	-1.667
Pt₃Co(511)	Edge	0.524	-1.530
Pt₃Co(511)	Terrace	0.599	-1.707
Pt₃Co(320)	Edge	0.105	-1.683
Pt₃Co(320)	Terrace	0.356	-1.820
Pt₃Co(332)	Edge	0.576	-1.671
Pt₃Co(332)	Terrace	0.723	-1.836

图S1 AIMD模拟过程中六个Pt3Co HIFs的温度、能量平衡曲线

Fig. S1 Temperature and energy balance curves during AIMD simulations of six Pt3Co HIFs (a) Pt3Co(211); (b) Pt3Co(310); (c) Pt3Co(331); (d) Pt3Co(511); (e) Pt3Co(320); (f) Pt3Co(332)

图S2 *O、*OH、*OOH在Pt3Co(211)台阶处的最佳吸附位点

Fig. S2 *O, *OH, and *OOH at the best adsorption sites of Pt3Co(211) terrace

图S3 *O、*OH、*OOH在Pt3Co(310)的最佳吸附位点

Fig. S3 *O, *OH, and *OOH at the best adsorption sites of Pt3Co(310) (a) Edge; (b) Terrace

图S4 *O、*OH、*OOH在Pt3Co(331)的最佳吸附位点

Fig. S4 *O, *OH, and *OOH at the best adsorption sites of Pt3Co(331) (a) Edge; (b) Terrace

图S5 *O、*OH、*OOH在Pt3Co(511)的最佳吸附位点

Fig. S5 *O, *OH, and *OOH at the best adsorption sites of Pt3Co(511) (a) Edge; (b) Terrace

图S6 *O、*OH、*OOH在Pt3Co(320)的最佳吸附位点

Fig. S6 *O, *OH, and *OOH at the best adsorption sites of Pt3Co(320) (a) Edge; (b) Terrace

图S7 *O、*OH、*OOH在Pt3Co(332)的最佳吸附位点

Fig. S7 *O, *OH, and *OOH at the best adsorption sites of Pt3Co(332) (a) Edge; (b) Terrace

图S8 六个HIFs在边缘、台阶1、台阶2处的ρdos和εd

Fig. S8 ρdos and εd for the six HIFs at edge, terrace 1, and terrace 2 (a1-a3) Pt3Co(211); (b1-b3) Pt3Co(310); (c1-c3) Pt3Co(331); (d1-d3) Pt3Co(511); (e1-e3) Pt3Co(320); (f1-f3) Pt3Co(332)

图S9 Pt3Co HIFs催化剂在边缘处的ORR自由能变化图

Fig. S9 Plots of ORR free energy at edge for Pt3Co HIFs catalysts (a) Pt3Co(211); (b) Pt3Co(310); (c) Pt3Co(331); (d) Pt3Co(511); (e) Pt3Co(320); (f) Pt3Co(332)

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Pt₃Co高指数晶面氧还原过程的密度泛函理论研究

Oxygen Reduction Reaction on Pt₃Co High-index Facets by Density Functional Theory

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