Pt-Cu合金催化剂上甲烷无氧偶联的机理与微观动力学研究: 从单原子位点到单团簇位点

doi:10.1016/S1872-2067(23)64408-0

催化学报 ›› 2023, Vol. 48: 90-100.DOI: 10.1016/S1872-2067(23)64408-0

Pt-Cu合金催化剂上甲烷无氧偶联的机理与微观动力学研究: 从单原子位点到单团簇位点

黄正清^a^,¹, 贺姝玥^a^,¹, 班涛^a, 高新^a, 许云华^b, 常春然^a^,^b^,^*()

^a西安交通大学化学工程与技术学院, 陕西省能源化工过程强化重点实验室, 陕西西安710049
^b榆林学院化学与化工学院, 陕西省低变质煤洁净利用重点实验室, 陕西榆林719000

收稿日期:2022-11-24 接受日期:2023-01-13 出版日期:2023-05-18 发布日期:2023-04-20
通讯作者: * 电子信箱: changcr@mail.xjtu.edu.cn (常春然).
作者简介:第一联系人：
¹共同第一作者
基金资助:
国家自然科学基金(22078257);国家自然科学基金(22108213);国家自然科学基金(22038011);国家自然科学基金(52176142);中国博士后科学基金(2021M692548);中国科学院洁净能源创新研究院-榆林学院联合基金(YLU-DNL Fund 2022001)

Mechanistic and microkinetic study of nonoxidative coupling of methane on Pt-Cu alloy catalysts: From single-atom sites to single-cluster sites

Zheng-Qing Huang^a^,¹, Shu-Yue He^a^,¹, Tao Ban^a, Xin Gao^a, Yun-Hua Xu^b, Chun-Ran Chang^a^,^b^,^*()

^aShaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi’an Jiaotong University, Xi’an 710049, Shaanxi, China
^bShaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization, School of Chemistry and Chemical Engineering, Yulin University, Yulin 719000, Shaanxi, China

Received:2022-11-24 Accepted:2023-01-13 Online:2023-05-18 Published:2023-04-20
Contact: * E-mail: changcr@mail.xjtu.edu.cn (C.-R. Chang).
About author:First author contact:
¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22078257);National Natural Science Foundation of China(22108213);National Natural Science Foundation of China(22038011);National Natural Science Foundation of China(52176142);China Postdoctoral Science Foundation(2021M692548);Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2022001)

摘要/Abstract

摘要：

随着天然气和页岩气资源的大量发现, 作为主要成分的甲烷, 其转化为高值化学品是一条具有开发潜力的路径. 在各种甲烷转化途径中, 甲烷无氧直接转化具有碳原子利用率高和二氧化碳排放少的优点, 更具应用前景. 然而, 甲烷的无氧转化仍然面临反应温度高、C₂烃选择性低和催化剂易积碳失活的难题. 因此, 大量的研究集中在催化剂研发上, 期望通过选择性地打破C-H键, 并且催化C-C偶联, 实现高效活化甲烷、高选择性生成C₂烃. 近期研究发现, 被Cu等金属隔离的Pt位点, 被金属氧化物分散的Pt位点, 都有利于甲烷无氧偶联生成C₂烃. 特别是Pt-Cu单原子合金催化剂, 其中分散的Pt单原子不仅具有较高的打破C-H键活性, 而且能够抑制甲烷深度脱氢, 具有很好的抗积碳性能. 虽然单原子Pt具有很好的甲烷活化性能, 但进一步催化C₂烃生成的反应过程并不清楚, 同时单分散的Pt团簇也可能存在于Pt-Cu合金表面, 而关于它们催化甲烷无氧偶联的机制也缺乏研究和认识.
本文在Cu(111)表面建立Pt₁, Pt₂和Pt₃位点(分别标记为Pt₁©Cu(111), Pt₂©Cu(111)和Pt₃©Cu(111)), 采用密度泛函理论计算与微观动力学模拟相结合的方法, 研究甲烷无氧偶联的催化反应机理与反应性能, 评估并比较单原子与单团簇的催化反应性能. 通过对甲烷分解的基元反应计算发现, CH₄, CH₃和CH₂的脱氢反应分别在Cu(111)上的Pt₁, Pt₂和Pt₃位点上最有利. 然而, 相应的CH_x (x = 3, 2, 1)物种直接偶联形成C₂H₆, C₂H₄和C₂H₂的反应, 分别在Cu(111)上的Pt₃, Pt₁和Pt₂位点上最有利. 三种Pt位点独特的反应趋势, 主要源于Pt位点与CH_x物种不同的结合能力. 反应条件下甲烷无氧偶联的微观动力学模拟表明, Pt₁©Cu(111)催化甲烷转化的活性最高, 而加入少量的氢气可以显著提高乙烯的选择性, 750 K时最高选择性可达96.2%. 在Pt₁©Cu(111)表面, Pt位点主要负责C-H键裂解, Cu位点是C-C偶联的活性中心. 通过密度泛函理论计算, 发现Pt₁©Cu(111)在反应条件下结构稳定. 综上, 本文揭示了Pt单原子位点(SASs)和Pt单团簇位点(SCSs)上的甲烷无氧偶联反应机制, 并预测Pt SASs在甲烷无氧偶联中比Pt SCSs更有优势, 为高效甲烷无氧偶联催化剂制备提供一定借鉴.

关键词: 甲烷, 微观动力学模拟, 单原子催化剂, 单团簇催化剂, 密度泛函理论

Abstract:

Desirable catalysts possessing the ability to selectively break C-H bond and controllably catalyze C-C bond formation are highly demanded for the nonoxidative coupling of methane (NOCM). Herein, a series of Pt-Cu alloy catalysts including Pt₁©Cu(111), Pt₂©Cu(111) and Pt₃©Cu(111) are deliberately designed and systematically studied for NOCM. Density functional theory calculations reveal that the Pt₁, Pt₂, and Pt₃ sites on Cu(111) can selectively break the C-H bond to generate CH₃, CH₂, and CH species, respectively. However, direct coupling of corresponding CH_x (x = 3, 2, 1) to form C₂H₆, C₂H₄, and C₂H₂ are favorable on Pt₃, Pt₁, and Pt₂ sites on Cu(111), respectively. The different reactivity trends of the three Pt sites mainly originate from the varying bonding abilities of CH_x species at the Pt sites. Microkinetic modeling manifests that the Pt₁©Cu(111) is the most active for methane dissociation (TOF = 2.98 s^-1 at 1000 K) and can selectively convert methane into ethylene with the highest selectivity up to 96.2% at 750 K. Moreover, Pt₁©Cu(111) also shows superb stability under reaction conditions. Overall, our studies not only provide a comprehensive understanding of the reaction mechanism of NOCM on Pt single-atom sites (SASs) and Pt single-cluster sites (SCSs) but also predict that Pt SASs are advantageous over Pt SCSs for NOCM.

Key words: Methane, Microkinetic modeling, Single-atom catalyst, Single-cluster catalyst, Density functional theory

黄正清, 贺姝玥, 班涛, 高新, 许云华, 常春然. Pt-Cu合金催化剂上甲烷无氧偶联的机理与微观动力学研究: 从单原子位点到单团簇位点[J]. 催化学报, 2023, 48: 90-100.

Zheng-Qing Huang, Shu-Yue He, Tao Ban, Xin Gao, Yun-Hua Xu, Chun-Ran Chang. Mechanistic and microkinetic study of nonoxidative coupling of methane on Pt-Cu alloy catalysts: From single-atom sites to single-cluster sites[J]. Chinese Journal of Catalysis, 2023, 48: 90-100.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64408-0

https://www.cjcatal.com/CN/Y2023/V48/I5/90

图/表 11

Fig. 1. Top views of the optimized structures of Pt1?Cu(111) (a), Pt2?Cu(111) (b), and Pt3?Cu(111) (c) surfaces. Only the first layer of the slab models is shown.

Fig. 2. Optimized structures of CH4 (a), CH3 (b), CH2 (c), CH (d), and C (e) adsorbed on the (111) surfaces of Pt1?Cu, Pt2?Cu, and Pt3?Cu, Cu, and Pt. The data without a bracket is the adsorption energy of CHx referring to the energy of CHx in the gas phase, whereas the data with a bracket is the adsorption energy of CHx referring to the energies of CH4 and H2 in the gas phase. The adsorption energies of CHx species and H atoms are also displayed in Table S1 and Fig. S1.

Fig. 3. (a) Linear scaling relationships between adsorption energies of CHx and that of C atom on the metal (111) surfaces of Pt1?Cu, Pt2?Cu, and Pt3?Cu, Cu, and Pt; (b) Intermediacy (α) of CHx adsorbed on the metal (111) surfaces. The fitting results and calculated intermediacies are listed in Tables S2 and S3, respectively. (c) The relative energy difference of CHx, ??E(CHx) = ?E(CHx) - ?E(CHx on Cu), on three Ptn?Cu catalysts referring to Cu. The energy difference of CHx is calculated as: ?E(CHx) = [E(CHx-1) - E(CHx)] - [E(CHx) - E(CHx+1)].

Fig. 4. (a) Energy profile of methane decomposition. (b) Br?nsted-Evans-Polanyi relations for methane decomposition on the metal (111) surfaces of Cu, Pt, Pt1?Cu, Pt2?Cu, and Pt3?Cu. The structures of corresponding intermediates are shown in Fig. 2 and the structures of corresponding transition states are displayed in Figs. S3 and S4.

Fig. 5. Optimized structures of transition states (TS) and final states (FS) in C-C coupling of two CH3 to form C2H6 (a), two CH2 to form C2H4 (b), and two CH to form C2H2 (c) on Pt1?Cu, Pt2?Cu, and Pt3?Cu (111) surfaces. The side-view structures are in the upper panel and the top-view structures are in the lower panel. The blue arrows in the top-view structure are the directions of the side-view structures.

Fig. 6. Br?nsted-Evans-Polanyi relations for CH3* coupling to form ethane (a), CH2* coupling to form ethylene (b), and CH* coupling to form acetylene (c).

Fig. 7. Reaction networks of nonoxidative coupling of methane to C2 hydrocarbons for microkinetic modeling. The asterisk (*) represents the Pt site, and the pound sign (#) represents the Cu site. The hydrogen involved in the reaction networks is not shown in this Figure.

Fig. 8. (a) TOF of methane consumption on (111) surfaces of Pt1?Cu, Pt2?Cu, Pt3?Cu and Cu. (b) Selectivity of C2H4 and C2H2 on (111) surfaces of Pt1?Cu, Pt2?Cu, and Pt3?Cu. The pressure of methane is 1.00 bar, and the pressures of other species are zero in (a) and (b). (c) TOF of methane consumption and selectivity of C2H6, C2H4 and C2H2 on Pt1?Cu(111). The data in solid dot is at P(CH4) = 1.00 bar, and P(H2) = 0.00 bar, and the data in hollow dot is at P(CH4) = 0.99 bar, and P(H2) = 0.01 bar.

Fig. 9. Advantageous reaction pathways of NOCM on Pt1?Cu(111) at 1000 K in pure methane [P(CH4) = 1.00 bar] (a) and in methane-hydrogen mixture [P(CH4) = 0.99 bar, P(H2) = 0.01 bar] (b). The numbers are the TOF in s-1 of corresponding elementary step. The elementary steps with TOF less than 10 s-1 in (a) and less than 0.10 s-1 in (b) are not listed in this Figure. The reactions represented by thicker red arrows are the advantageous pathways. (c) Degree of rate control analysis on methane consumption under different reaction conditions. (d) Degree of selectivity control analysis on ethylene production under different reaction conditions. States with absolute values greater than 0.02 in (c) and (d) are shown. The reaction rates of all the elementary steps and the labels representing the states are listed in Table S7.

Fig. 10. (a) First-principle energy of a nine-layer (3 × 3) Cu slab with one Cu atom replaced by a Pt atom in a vacuum or adsorbed by CH3, C, or H atom. The zero-energy reference is the Pt atom in the first atom layer of the Cu slab. (b) The top-view and side-view structures of the Cu slab with one Cu atom replaced by a Pt atom adsorbed by CH3, C, or H atom.

Fig. 11. (a) First-principle energy of transformation from two isolated Pt atoms to one Pt dimer in a vacuum or adsorbed by CH3, C, or H atom. (b) First-principle energy of the transformation from three isolated Pt atoms to one Pt trimer in a vacuum or adsorbed by CH3, C, or H atom.

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Pt-Cu合金催化剂上甲烷无氧偶联的机理与微观动力学研究: 从单原子位点到单团簇位点

Mechanistic and microkinetic study of nonoxidative coupling of methane on Pt-Cu alloy catalysts: From single-atom sites to single-cluster sites

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