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学者姓名：林森
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The local structure of the metal single-atom site is closely related to the catalytic activity of metal single-atom catalysts(SACs).However,constructing SACs with homogeneous metal active sites is a challenge due to the surface heterogeneity of the conventional support.Herein,we prepared two Rh1/CeO2 SACs(0.5Rh1/r-CeO2 and 0.5Rh1/c-CeO2,respectively)using two shaped CeO2(rod and cube)exposing different facets,i.e.,CeO2(111)and CeO2(100).In CO oxidation reaction,the T100 of 0.5Rh1/r-CeO2 SACs is 120 ℃,while the T100 of 0.5Rh1/c-CeO2 SACs is as high as 200 ℃.Via in-situ CO diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS),we found that the proximity between OH group and Rh single atom on the plane surface plays an important role in the catalytic activity of Rh1/CeO2 SAC system in CO oxidation.The Rh single atom trapped at the CeO2(111)crystal surface forms the Rh1(OH)adjacent species,which is not found on the CeO2(100)crystal surface at room temperature.Furthermore,during CO oxidation,the OH group far from Rh single atom on the 0.5Rh1/c-CeO2 disappears and forms Rh1(OH)adjacent species when the temperature is above 150 ℃.The formation of Rh1(OH)adjacentCO intermediate in the reaction is pivotal for the excellent catalytic activity,which explains the difference in the catalytic activity of Rh single atoms on two different CeO2 planes.The formed Rh1(OH)adjacent-O-Ce structure exhibits good stability in the reducing atmosphere,maintaining the Rh atomic dispersion after CO oxidation even when pre-reduced at high temperature of 500 ℃.Density functional theory(DFT)calculations validate the unique activity and reaction path of the intermediate Rh1(OH)adjacentCO species formed.This work demonstrates that the proximity between metal single atom and hydroxyl can determine the formation of active intermediates to affect the catalytic performances in catalysis.
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| GB/T 7714 | Danfeng Wu , Shuyun Zhou , Congcong Du et al. The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO2 single-atom catalysts [J]. | 纳米研究（英文版） , 2024 , 17 (1) : 397-406 . |
| MLA | Danfeng Wu et al. "The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO2 single-atom catalysts" . | 纳米研究（英文版） 17 . 1 (2024) : 397-406 . |
| APA | Danfeng Wu , Shuyun Zhou , Congcong Du , Juan Li , Jianyu Huang , Hong-xia Shen et al. The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO2 single-atom catalysts . | 纳米研究（英文版） , 2024 , 17 (1) , 397-406 . |
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Graphitic carbon nitride (g-C3N4), recognized for its considerable potential as a heterogeneous photocatalyst in water splitting, has attracted extensive research interest. By using density functional theory (DFT) calculations, the regulatory role of p-block metal (PM) single atoms on the photocatalytic activity of g-C3N4 in overall water splitting was systematically explored. The incorporation of PM atoms (Ge, Sn and Pb) led to a reduction in the overpotentials required for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER). Combined with the electronic structures analysis via hybrid functional, it was found that the introduction of Ge, Sn or Pb optimizes the positions of the valence band maximum (VBM) and the conduction band minimum (CBM), providing a robust driving force for HER and ensuring substantial driving force for OER. Meanwhile, the presence of these three PMs induces the spatial separation of VBM and CBM, inhibiting the recombination of carriers. These findings have significant implications for the design and preparation of efficient photocatalysts.
Keyword ：
DFT DFT graphitic carbon nitride graphitic carbon nitride p-block metal p-block metal semiconductor photocatalysis semiconductor photocatalysis water splitting water splitting
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| GB/T 7714 | Chen, Mengning , Wu, Yidi , Wan, Qiang et al. Theoretical Study of p-Block Metal Single-Atom-Loaded Carbon Nitride Catalyst for Photocatalytic Water Splitting [J]. | MOLECULES , 2024 , 29 (9) . |
| MLA | Chen, Mengning et al. "Theoretical Study of p-Block Metal Single-Atom-Loaded Carbon Nitride Catalyst for Photocatalytic Water Splitting" . | MOLECULES 29 . 9 (2024) . |
| APA | Chen, Mengning , Wu, Yidi , Wan, Qiang , Lin, Sen . Theoretical Study of p-Block Metal Single-Atom-Loaded Carbon Nitride Catalyst for Photocatalytic Water Splitting . | MOLECULES , 2024 , 29 (9) . |
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Spillover of adsorbed species from one active site to another is a key step in heterogeneous catalysis. However, the factors controlling this step, particularly the spillover of polyatomic species, have rarely been studied. Herein, we investigate the spillover dynamics of H* and CH3* species on a single-atom alloy surface (Rh/Cu(111)) upon the dissociative chemisorption of methane (CH4), using molecular dynamics that considers both surface phonons and electron-hole pairs. These dynamical calculations are made possible by a high-dimensional potential energy surface machine learned from density functional theory data. Our results provide compelling evidence that the H* and CH3* can spill over on the metal surface at experimental temperatures and reveal novel dynamical features involving an internal motion during diffusion for CH3*. Increasing surface temperature has a minor effect on promoting spillover, as geminate recombinative desorption becomes more prevalent. However, the poisoning of the active site can be mitigated by the frequent gaseous molecular collisions that occur under ambient pressure in real-world catalysis, which transfer energy to the trapped adsorbates. Interestingly, the bulky CH3* exhibits a significant spillover advantage over the light H* due to its larger size, which facilitates energy acquisition. These insights help to advance our understanding of spillover in heterogeneous catalysis. © 2024 Wiley-VCH GmbH.
Keyword ：
Gaseous molecular collisions Gaseous molecular collisions machine learning machine learning molecular dynamics molecular dynamics potential energy surface potential energy surface spillover spillover
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| GB/T 7714 | Gu, K. , Guo, H. , Lin, S. . Deciphering the Factors Controlling Hydrogen and Methyl Spillover upon Methane Dissociation on Rh/Cu(111) Single-Atom Alloy [J]. | Angewandte Chemie - International Edition , 2024 , 63 (39) . |
| MLA | Gu, K. et al. "Deciphering the Factors Controlling Hydrogen and Methyl Spillover upon Methane Dissociation on Rh/Cu(111) Single-Atom Alloy" . | Angewandte Chemie - International Edition 63 . 39 (2024) . |
| APA | Gu, K. , Guo, H. , Lin, S. . Deciphering the Factors Controlling Hydrogen and Methyl Spillover upon Methane Dissociation on Rh/Cu(111) Single-Atom Alloy . | Angewandte Chemie - International Edition , 2024 , 63 (39) . |
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Single-atom catalysts (SACs) are emerging as promising candidates for electrochemical nitrogen reduction reaction (NRR). Previous studies have shown that the single-atom centers of SACs can not only serve as active sites, but also act as promoters to affect the catalytic properties. However, the use of single metal atoms as promoters in electrocatalysis has rarely been studied. In this work, the defective Keggin-type phosphomolybdic acid (PMA) is used as a substrate to support the single metal atoms. We aim to tune the electronic structures of the exposed molybdenum active sites on defective PMA by using these supported single atoms as promoters for efficient NRR. Firstly, the stability and N2 adsorption capacity were studied to screen for an effective catalyst capable of activating N2. Most of the SACs were found to have good stability and N2 adsorption capacity. Then, we compared the selectivity and NRR activity of the catalysts and found that catalysts with metal atom promoters have improved NRR selectivity and activity. Finally, electronic structure analysis was carried out to understand the promoting effect of the promoter on N2 activation and the activity of the NRR process. This work provides a new strategy for designing efficient catalysts for electrocatalytic reactions by introducing promoters. A new strategy is proposed for designing efficient catalysts for electrocatalytic nitrogen reduction by introducing single atom promoters.
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| GB/T 7714 | Lin, Linghui , Ma, Ruijie , Jiang, Rong et al. Design of high performance nitrogen reduction electrocatalysts by doping defective polyoxometalate with a single atom promoter [J]. | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2024 , 26 (10) : 8494-8503 . |
| MLA | Lin, Linghui et al. "Design of high performance nitrogen reduction electrocatalysts by doping defective polyoxometalate with a single atom promoter" . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS 26 . 10 (2024) : 8494-8503 . |
| APA | Lin, Linghui , Ma, Ruijie , Jiang, Rong , Lin, Sen . Design of high performance nitrogen reduction electrocatalysts by doping defective polyoxometalate with a single atom promoter . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2024 , 26 (10) , 8494-8503 . |
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Adsorbates on metal surfaces are typically formed from the dissociative chemisorption of molecules occurring at gas-solid interfaces. These adsorbed species exhibit unique diffusion behaviors on metal surfaces, which are influenced by their translational energy. They play crucial roles in various fields, including heterogeneous catalysis and corrosion. This review examines recent theoretical advancements in understanding the diffusion dynamics of adsorbates on metal surfaces, with a specific emphasis on hydrogen and oxygen atoms. The diffusion processes of adsorbates on metal surfaces involve two energy transfer mechanisms: surface phonons and electron-hole pair excitations. This review also surveys new theoretical methods, including the characterization of the electron-hole pair excitation within electronic friction models, the acceleration of quantum chemistry calculations through machine learning, and the treatment of atomic nuclear motion from both quantum mechanical and classical perspectives. Furthermore, this review offers valuable insights into how energy transfer, nuclear quantum effects, supercell sizes, and the topography of potential energy surfaces impact the diffusion behavior of hydrogen and oxygen species on metal surfaces. Lastly, some preliminary research proposals are presented. This review examines recent theoretical advancements in understanding the diffusion dynamics of adsorbates on metal surfaces, with a specific emphasis on hydrogen and oxygen atoms. It offers valuable insights into how energy transfer, nuclear quantum effects, supercell sizes, and the topography of potential energy surfaces impact the diffusion behavior of these two species. image
Keyword ：
Electron-hole pairs excitation Electron-hole pairs excitation machine learning machine learning molecular dynamics molecular dynamics potential energy surface potential energy surface spillover spillover
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| GB/T 7714 | Gu, Kaixuan , Lin, Sen . Advances in the Dynamics of Adsorbate Diffusion on Metal Surfaces: Focus on Hydrogen and Oxygen [J]. | CHEMPHYSCHEM , 2024 , 25 (12) . |
| MLA | Gu, Kaixuan et al. "Advances in the Dynamics of Adsorbate Diffusion on Metal Surfaces: Focus on Hydrogen and Oxygen" . | CHEMPHYSCHEM 25 . 12 (2024) . |
| APA | Gu, Kaixuan , Lin, Sen . Advances in the Dynamics of Adsorbate Diffusion on Metal Surfaces: Focus on Hydrogen and Oxygen . | CHEMPHYSCHEM , 2024 , 25 (12) . |
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Despite extensive studies of hydrogen spillover on single-atom alloy surfaces, a thorough understanding of the structure-activity relationship is still lacking. Here, we investigate H-2 dissociation and diffusion of the dissociated H species on the near-surface alloys embedded with single Pt atoms using density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations. The DFT results indicate that subsurface alloying with early transition metals (X) (Pt1-X/Cu(111)) can generally promote the initial hydrogen spillover but suppress the H-2 dissociation process, showing an intractable trade-off effect. While the DFT-calculated H-2 dissociation barrier on Pt-1-Co/Cu(111) is higher than that on Pt-1-Ni/Cu(111), the AIMD results show that the H-2 dissociation probability on the Pt-1-Co/Cu(111) surface is much higher than that on Pt1-Ni/Cu(111). The trajectory analysis shows that H-2 molecules on Pt-1-Co/Cu(111) can adopt a more convenient conformation for dissociation when approaching the so-called close-range physisorption zone (CPZ) due to the relatively flat topography of the potential energy surface, thus increasing the H-2 dissociation probability compared to the case on Pt-1-Ni/Cu(111). This work provides a clear picture for understanding the structure-activity relationships of H-2 activation and hydrogen spillover over single-atom catalysts. More importantly, it highlights an overlooked but essential role of the dynamic orientation of the reactant in heterogeneous catalysis.
Keyword ：
ab initio molecular dynamics ab initio molecular dynamics density functional theory density functional theory H-2 dissociation H-2 dissociation hydrogen spillover hydrogen spillover single-atom catalysis single-atom catalysis
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| GB/T 7714 | Tan, Zhenghui , Chen, Jun , Lin, Sen . Theoretical Insights into H2 Activation and Hydrogen Spillover on Near-Surface Alloys with Embedded Single Pt Atoms [J]. | ACS CATALYSIS , 2024 , 14 (4) : 2194-2201 . |
| MLA | Tan, Zhenghui et al. "Theoretical Insights into H2 Activation and Hydrogen Spillover on Near-Surface Alloys with Embedded Single Pt Atoms" . | ACS CATALYSIS 14 . 4 (2024) : 2194-2201 . |
| APA | Tan, Zhenghui , Chen, Jun , Lin, Sen . Theoretical Insights into H2 Activation and Hydrogen Spillover on Near-Surface Alloys with Embedded Single Pt Atoms . | ACS CATALYSIS , 2024 , 14 (4) , 2194-2201 . |
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As COVID-19 coexists with humans, the need for home oxygen (O2) generators has grown, especially for those with heart and lung conditions. This study presents a prototype of an electrolyte-free proton-exchange membrane electrochemical oxygen generator (EOG) that uses pure water for safe, high-performance operation. The development of a novel oxygen evolution reaction catalyst, PtxIryRu1-x-yO2, and an efficient membrane electrode assembly has improved the EOG's performance, achieving a 1 L min−1 oxygen production rate and over 600 h of stability. Furthermore, the EOG demonstrates several distinct advantages for medical applications, including (1) directly producing sterile and medical-grade O2 (purity >99.5%), (2) supporting nearly instantaneous O2 supply for emergency (startup time <1 s), (3) supporting portable application due to its light weight (<2 kg) and compact size (1 dm3), and (4) ensuring a quiet operating condition for patients (<45 dB). The EOG, boasting unique application advantages, significantly outperforms commercial pressure swing adsorption devices, thereby showcasing its considerable potential for future applications. © 2024 The Authors
Keyword ：
DTI-3: Develop DTI-3: Develop electrochemical oxygen production electrochemical oxygen production EOG EOG household application household application OER OER oxygen generators oxygen generators
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| GB/T 7714 | Zhao, X. , Zhao, J. , Li, D. et al. Electrolyte-free electrochemical oxygen generator for providing sterile and medical-grade oxygen in household applications [J]. | Device , 2024 , 2 (9) . |
| MLA | Zhao, X. et al. "Electrolyte-free electrochemical oxygen generator for providing sterile and medical-grade oxygen in household applications" . | Device 2 . 9 (2024) . |
| APA | Zhao, X. , Zhao, J. , Li, D. , Zhou, F. , Li, P. , Tan, Y. et al. Electrolyte-free electrochemical oxygen generator for providing sterile and medical-grade oxygen in household applications . | Device , 2024 , 2 (9) . |
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Hydrogen peroxide (H2O2) is an important chemical with a diverse range of industrial applications in chemical synthesis and medical disinfection. The traditional anthraquinone oxidation process, with high energy consumption and complexity, is being replaced by cost-effective and environmentally friendly alternatives. In order to explore suitable catalysts for the electrocatalytic synthesis of H2O2, the stability of B,N-doped graphene loaded with various p-block metal (PM) single atoms (i.e., PM-NxBy: x and y represent the number of atoms of N and B, respectively) and the effects of different numbers and positions of B dopants in the second coordination shell on the catalytic performance were studied by density functional theory (DFT) calculations. The results show that Ga-N4B6 and Sb-N4B6 exhibit enhanced stability and 2e− oxygen reduction reaction (ORR) activity and selectivity. Their thermodynamic overpotential η values are 0.01 V, 0.03 V for Ga-N4B6’s two configurations and 0.02 V, 0 V for Sb-N4B6’s two configurations. Electronic structure calculations indicate that the PM single atom adsorbs OOH* intermediates and transfers electrons into them, resulting in the activation of the O-O bond, which facilitates the subsequent hydrogenation reaction. In summary, Sb-N4B6 and Ga-N4B6 exhibit extraordinary 2e− ORR performance, and their predicted activities are comparable to those of known outstanding catalysts (such as PtHg4 alloy). We propose effective strategies on how to enhance the 2e− ORR activities of carbon materials, elucidate the origin of the activity of potential catalysts, and provide insights for the design and development of electrocatalysts that can be used for H2O2 production. © 2024 by the authors.
Keyword ：
2e− ORR 2e− ORR electrocatalysis electrocatalysis p-block metal single atom p-block metal single atom
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| GB/T 7714 | Wu, Y. , Zhang, Y. , Lin, S. . Effect of the Second-Shell Coordination Environment on the Performance of P-Block Metal Single-Atom Catalysts for the Electrosynthesis of Hydrogen Peroxide [J]. | Catalysts , 2024 , 14 (7) . |
| MLA | Wu, Y. et al. "Effect of the Second-Shell Coordination Environment on the Performance of P-Block Metal Single-Atom Catalysts for the Electrosynthesis of Hydrogen Peroxide" . | Catalysts 14 . 7 (2024) . |
| APA | Wu, Y. , Zhang, Y. , Lin, S. . Effect of the Second-Shell Coordination Environment on the Performance of P-Block Metal Single-Atom Catalysts for the Electrosynthesis of Hydrogen Peroxide . | Catalysts , 2024 , 14 (7) . |
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For single-atom catalysts (SACs), the dopants situated near the metal site have demonstrated a significant impact on the catalytic properties. However, the effect of dopants situated further away from the metal centers and their working mechanisms remain to be elucidated. Herein, we conduct density functional theory-driven studies on regulating the peripheral nitrogen dopants in graphene-based SACs, with a particular focus on Ir1 SAC, for propane dehydrogenation (PDH). It is found that increasing the distance between the N dopant and the Ir1 site results in a different energy change for the reaction process compared to the dense doping models with only first and second-shell N species. The proposed stochastic doping models demonstrate statistically that increasing the N dopant in farther shells not only enhances the activity of Ir1 but also maintains a high selectivity for propene, which is verified by experimental tests. The modulation of the d-band center of Ir1 by stochastic N dopants effectively modifies the binding strength of reaction intermediates, thereby enabling the optimization of the potential energy surface of PDH. These results deepen the understanding of dopant states around metal sites and provide an important implication for the doping engineering in heterogeneous catalysis. © 2024 Wiley-VCH GmbH.
Keyword ：
iridium iridium peripheral effect peripheral effect propane dehydrogenation propane dehydrogenation reactivity reactivity Single-atom catalysts Single-atom catalysts
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| GB/T 7714 | Wei, F. , Cao, L. , Ge, B. et al. Regulating Peripheral Nitrogen Dopants in Single-Atom Catalysts to Enhance Propane Dehydrogenation [J]. | Angewandte Chemie - International Edition , 2024 , 64 (5) . |
| MLA | Wei, F. et al. "Regulating Peripheral Nitrogen Dopants in Single-Atom Catalysts to Enhance Propane Dehydrogenation" . | Angewandte Chemie - International Edition 64 . 5 (2024) . |
| APA | Wei, F. , Cao, L. , Ge, B. , Chen, Y. , Pan, X. , Chai, Y. et al. Regulating Peripheral Nitrogen Dopants in Single-Atom Catalysts to Enhance Propane Dehydrogenation . | Angewandte Chemie - International Edition , 2024 , 64 (5) . |
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Developing active, stable, and cost-efficient electrocatalysts to replace platinum for the alkaline hydrogen evolution reaction (HER) is highly desirable yet represents a great challenge. Here, it is reported on a facile one-pot synthesis of RuxNi layered double hydroxides (RuxNi-LDHs) that exhibit remarkable HER activity and stability after an in-situ activation treatment, surpassing most state-of-the-art Ru-based catalysts as well as commercial Ru/C and Pt/C catalysts. The structural and chemical changes triggered by in-situ activation are systematically investigated, and the results clearly show that the pristine, less-active RuxNi-LDHs are transformed into a highly active catalyst characterized by raft-like, defect-rich Ru degrees particles decorated on the surface of RuxNi-LDHs. Density functional theory (DFT) calculations reveal that the defective Ru sites can effectively optimize the reaction pathway and lower the free energies of the elemental steps involved, leading to enhanced intrinsic activity. This work highlights the importance of the currently understudied strategy of defect engineering in boosting the HER activity of Ru-based catalysts and offers an effective approach involving in-situ electrochemical activation for the development of high-performance alkaline HER catalysts.
Keyword ：
alkaline HER alkaline HER defect engineering defect engineering defective Ru-degrees NPs defective Ru-degrees NPs first-principles calculations first-principles calculations RuxNi-LDHs RuxNi-LDHs
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| GB/T 7714 | Shi, Ningning , Ma, Ruijie , Lin, Linghui et al. In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution [J]. | SMALL , 2024 , 20 (27) . |
| MLA | Shi, Ningning et al. "In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution" . | SMALL 20 . 27 (2024) . |
| APA | Shi, Ningning , Ma, Ruijie , Lin, Linghui , Xie, Wangjing , Liu, Panpan , Li, Peng et al. In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution . | SMALL , 2024 , 20 (27) . |
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