基于铁电In2Se3极化切换的N2还原单原子催化剂

doi:10.1016/S1872-2067(24)60084-7

催化学报 ›› 2024, Vol. 63: 244-257.DOI: 10.1016/S1872-2067(24)60084-7

基于铁电In₂Se₃极化切换的N₂还原单原子催化剂

穆楠^a, 薄婷婷^a, 胡玉高^a, 徐瑞欣^a, 刘彦昱^b^,^*(), 周伟^a^,^*()

^a天津大学理学院物理系, 天津市低维功能材料物理与制备技术重点实验室, 天津 300072
^b天津师范大学物理与材料科学学院, 天津 300387

收稿日期:2024-05-07 接受日期:2024-06-24 出版日期:2024-08-18 发布日期:2024-08-19
通讯作者: *电子信箱: yyliu@tjnu.edu.cn (刘彦昱),weizhou@tju.edu.cn (周伟).
基金资助:
国家自然科学基金(51972227);天津大学研究生文理拔尖创新奖励计划(B2-2023-005)

Single-atom catalysts based on polarization switching of ferroelectric In₂Se₃ for N₂ reduction

Nan Mu^a, Tingting Bo^a, Yugao Hu^a, Ruixin Xu^a, Yanyu Liu^b^,^*(), Wei Zhou^a^,^*()

^aDepartment of Physics, Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology, School of Science, Tianjin University, Tianjin 300072, China
^bCollege of Physics and Materials Science, Tianjin Normal University, Tianjin 300387, China

Received:2024-05-07 Accepted:2024-06-24 Online:2024-08-18 Published:2024-08-19
Contact: *E-mail: yyliu@tjnu.edu.cn (Y. Liu), weizhou@tju.edu.cn (W. Zhou).
Supported by:
National Natural Science Foundation of China(51972227);Arts and Science Excellence and Innovation Award Program for Graduate Student of Tianjin University(B2-2023-005)

摘要/Abstract

摘要：

氨(NH₃)作为反应物广泛应用于化学品、化肥等生产, 且随着工业快速发展, 其需求量不断增加. 目前, 工业合成NH₃主要依赖于传统的Haber-Bosch工艺, 但该工艺需要严苛的条件(500 °C和300 atm), 不仅能源消耗量大, 还排放大量温室气体. 因此, 寻找绿色NH₃合成技术以应对能源和环境挑战迫在眉睫. 受固氮酶技术启发, 利用N₂和H₂O进行氮还原反应(NRR)合成NH₃因能量消耗少和无污染等特点而备受关注. 然而, 析氢反应(HER)作为主要竞争反应严重影响NRR反应效率, 因此, 如何提升NRR反应活性和选择性至关重要.

本文提出了在铁电材料In₂Se₃上锚定过渡金属原子(TM@In₂Se₃)以形成活性中心, 并考察了极化取向对NRR的影响. 通过结合能、分子动力学和布拜图证明了TM@In₂Se₃体系的稳定性. 利用光谱嵌入和多维缩放(MDS)算法可视化研究了过渡金属原子的特征相似程度, K-means分组结果表明, 引入同组或临近过渡金属的TM@In₂Se₃体系往往具有相近的性能, 如结合能和NRR反应限制势等. 在极化切换过程中, 表面静电势的差异使得电子态重新分布, 这影响了吸附的小分子和催化剂基底之间的相互作用, 进而改变了反应屏障. NRR和HER的热力学自由能结果表明, V原子锚定在极化向下方向的In₂Se₃(V@↓-In₂Se₃)等体系具有较低的限制势和100%的理论法拉第效率. 相较于↑-In₂Se₃, ↓-In₂Se₃抑制了*H的吸附, 进而提升了NRR选择性. 态密度研究结果揭示了差异原因, 在极化向下切换为极化向上过程中, 作为活性位点的过渡金属原子的E(d_z₂)态能级提升, 改变了H-s和N-2p态与其轨道波函数的空间最大重叠, 使得极化切换能够控制催化反应类型进而得到不同的反应产物(决定了反应更利于析氢反应还是氮还原反应, 产物是氢气还是NH₃). 能带图结果表明, TM@In₂Se₃表现出局域的金属性, 同时通过电导率与I-V曲线对比了两个极化方向的电学特性, 过渡态的较低势垒证明了V@In₂Se₃在实验中能够实现铁电极化翻转. 晶体轨道哈密顿布居函数、随机森林算法和良好拟合关系也都验证了d电子与催化性能密切相关, 能够作为NRR反应限制势的描述符. 此外, 确定独立性筛选与稀疏化算子给出了基于特征组成的新描述符. 电子局域函数和差分电荷密度表明, 锚定过渡金属是有效激活N₂的策略. 结合表面状态(*O、*OH和*H的吸附)、布拜图和分子动力学结果, 证明了V@↓-In₂Se₃具有较好的N₂选择性、高的电化学和热力学稳定性.

综上, 本文发展了一种在In₂Se₃上锚定过渡金属原子调控催化性能的策略, 可以有效降低NRR反应过程限制势, 同时极化切换能够调控NRR和HER反应开关, 为设计高性能可调控的双功能催化剂提供参考.

关键词: 三硒化二铟单层, 密度泛函理论, 铁电切换, 单原子催化剂, 氮还原反应, 机器学习

Abstract:

The polarization switching plays a crucial role in controlling the final products in the catalytic process. The effect of polarization orientation on nitrogen reduction was investigated by anchoring transition metal atoms to form active centers on ferroelectric material In₂Se₃. During the polarization switching process, the difference in surface electrostatic potential leads to a redistribution of electronic states. This affects the interaction strength between the adsorbed small molecules and the catalyst substrate, thereby altering the reaction barrier. In addition, the surface states must be considered to prevent the adsorption of other small molecules (such as *O, *OH, and *H). Furthermore, the V@↓-In₂Se₃ possesses excellent catalytic properties, high electrochemical and thermodynamic stability, which facilitates the catalytic process. Machine learning also helps us further explore the underlying mechanisms. The systematic investigation provides novel insights into the design and application of two-dimensional switchable ferroelectric catalysts for various chemical processes.

Key words: In₂Se₃ monolayer, Density functional theory, Ferroelectric switching, Single atom catalysts, Nitrogen reduction reaction, Machine learning

穆楠, 薄婷婷, 胡玉高, 徐瑞欣, 刘彦昱, 周伟. 基于铁电In₂Se₃极化切换的N₂还原单原子催化剂[J]. 催化学报, 2024, 63: 244-257.

Nan Mu, Tingting Bo, Yugao Hu, Ruixin Xu, Yanyu Liu, Wei Zhou. Single-atom catalysts based on polarization switching of ferroelectric In₂Se₃ for N₂ reduction[J]. Chinese Journal of Catalysis, 2024, 63: 244-257.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(24)60084-7

https://www.cjcatal.com/CN/Y2024/V63/I8/244

图/表 13

Fig. 1. (a) The top and side views of geometric structures of the α-In2Se3 monolayer with downward and upward polarization, respectively. Purple and green denote the In atom and Se atom, respectively. The red cycles, blue cycles, and black arrows represent selected TM anchored sites, different Se atoms, and polarization directions, respectively. (b) The partial density of states of the α-In2Se3 monolayer with spin up state. (c) The average potential energy for In2Se3 monolayer along the perpendicular direction. The black arrow represents the direction of the intrinsic electric field. (d) The partial density of states and labelled p band centers of V@↓-In2Se3 and V@↑-In2Se3.

Fig. 2. Dimensionality reduction for the binding energy of the TM@In2Se3 using multidimensional scaling (a) and spectral embedding algorithms (b).

Fig. 3. (a) Schematic of Distal, Alternating and Enzymatic Mechanisms for NRR. (b) Proposed screening strategy of NRR candidate catalysts. (c) N2 absorption free energies with end-on and side-on patterns. (d) The bonding schematic diagrams between N2 and TM. (e) The N-N bond length changes as a function of the excess electrons after N2 adsorption for TM@↑-In2Se3 and TM@↓-In2Se3 via the end-on configuration.

Fig. 4. Free energy changes of *N2 + H+ + e- → *N2H (a) and *NH2 + H+ + e- → *NH3 (b) on TM@↑-In2Se3 with end-on configuration. Free energy changes of *N2 + H+ + e- → *N2H and *NH2 + H+ + e- → *NH3 on TM@↓-In2Se3 with end-on configuration (c) and on TM@↑-In2Se3 with side-on configuration (d). (e) The Gibbs free energy change of PDS for TM@In2Se3. (f) The limiting potentials for NRR and HER of TM@In2Se3 via Distal pathway, Alternating pathway, and Enzymatic pathway.

Fig. 5. (a) The electrical conductivity of the V@In2Se3. (b) The calculated I-V curve for the V@In2Se3.

Fig. 6. The Free energy diagrams during the NRR on V@↓-In2Se3 (a) and V@↑-In2Se3 (b) via distal pathway. Gibbs free energy diagram of the HER on V@↓-In2Se3 (c), V@↑-In2Se3 (d), Mo@↓-In2Se3 (e), Mo@↑-In2Se3 (f).

Fig. 7. The partial density of states of V-3d on the V@↓-In2Se3 (a) and V@↑-In2Se3 (b). (c) Schematic diagram of TM-d orbitals splitting in the different crystal fields. The partial density of states of Mo-4d on the Mo@↓-In2Se3 (d) and Mo@↑-In2Se3 (e). (f) Schematic diagram of the crystal field effect between the dz2 orbital of V atom and the ligand of Se atoms with the FE polarization switching.

Fig. 8. (a) Schematics of N atomic orbitals and N2 molecular orbitals. (b) The partial density of states of free N2. The partial density of states and crystal orbital Hamilton populations of N2 on V@↓-In2Se3 (c) and V@↑-In2Se3 (d) via end-on configuration. The bonding and antibonding states are depicted by cyan and yellow, respectively.

Fig. 9. (a) Interaction diagram between the 2p orbital of N atom and the d orbital of the TM atom with end-on configuration. (b) Important features from the Random Forest model for ΔG*NNH. (c) The linear correlations between the d band center (εd) of TM atom and limiting potential by the distal mechanism on TM@In2Se3. (d) The linear correlations between the excess obtained electrons of N2 and limiting potential by the distal mechanism on TM@In2Se3. (e) Comparison of DFT-calculated UL values with the SISSO-predicted values.

Fig. 10. The configuration and ELF maps of V@↓-In2Se3 (a), *NN (end-on pattern) (b) and *NH2 on V@↓-In2Se3 (c).

Fig. 11. (a) The differential charge density plots of N2 adsorbed on V@↓-In2Se3 and V@↑-In2Se3. (b) The schematic diagram of three moieties on TM@In2Se3: moieties 1, 2, and 3 represent In2Se3, single TM atom, and adsorbed NxHy, respectively. The charge variations of the three moieties for the NRR on V@↓-In2Se3 (c) and V@↑-In2Se3 (d).

Fig. 12. Surface Pourbaix diagrams of V@↓-In2Se3 (a) and V@↑-In2Se3 (c); Competitive adsorption of *N2 and *H as well as *OH and *O at the V site on V@↓-In2Se3 (b) and V@↑-In2Se3 (d) as a function of electrode potential.

Fig. 13. Pourbaix diagrams (a) and the AIMD simulation (b) of V@↓-In2Se3.

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基于铁电In₂Se₃极化切换的N₂还原单原子催化剂

Single-atom catalysts based on polarization switching of ferroelectric In₂Se₃ for N₂ reduction

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