Ultralow-temperature photochemical synthesis of atomically dispersed Pt catalysts for the hydrogen evolution reaction

Wei, Hehe; Wu, Hongbo; Huang, Kai; Ge, Binghui; Ma, Jingyuan; Lang, Jialiang; Zu, Di; Lei, Ming; Yao, Yugui; Guo, Wei; Wu, Hui

doi:10.1039/c8sc04986f

Cited by 89 publications

(72 citation statements)

References 44 publications

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“…The enhanced performance of Pt SACs compared to bulk Pt results from the charge transfer from Pt to adjacent C/N atoms, as reflected in the higher oxidation state of Pt in XANES and the Bader charge analysis, which leads to the change of unoccupied d orbitals of single Pt atoms, favoring the HER process . Interestingly, HER free energy diagrams of PtN x sites reveal that the binding strength of H* is weakened with an increase in H coverage of the Pt atom surface . Thus, simultaneously binding two or more H atoms on a single Pt atom to catalyze the HER process follows the Tafel mechanism.…”

Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

“…Since Pt is highly stable in both acids and bases, it is difficult to isolate single Pt atoms by removing Pt clusters and nanoparticles through traditional acid‐leaching methods. Thus, several vacancy trapping methods have been developed to prepare atomically dispersed PtC x and PtN x sites, which exhibit lower overpotentials, a smaller Tafel slope, and offer considerably higher stability compared to that of the commercial Pt/C catalyst. The enhanced performance of Pt SACs compared to bulk Pt results from the charge transfer from Pt to adjacent C/N atoms, as reflected in the higher oxidation state of Pt in XANES and the Bader charge analysis, which leads to the change of unoccupied d orbitals of single Pt atoms, favoring the HER process .…”

Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

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Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

282

240

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Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.

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Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

282

240

View full text Add to dashboard Cite

show abstract

“…[90,91] According to previous literatures, many synthetic techniques have been documented for downscaling metal NPs on the support, such as thermal decomposition and iced-photochemical reduction methods. [92][93][94] Through thermal decomposition, Corma and coworkers successfully realized the transformation from Pt NPs to single Pt atoms by O 2 activation ( Figure 1). [93] It has been demonstrated that the resultant single-atom Pt can obviously enhance the reaction kinetics due to the high dispersion of isolated Pt atoms on high-silica chabazite.…”

Section: Transforming Nps and Clusters To Single Atomsmentioning

confidence: 99%

“…Wu et al also found that the iced-photochemical technique exhibited great potential in downsizing metal NPs. [94] As compared with the conventional photochemical method, this novel synthesis technique can well fragment metal NPs into smaller NPs and even atomically dispersed metals, which would occupy a vitally important status in the fabrication of efficient and durable SACs.…”

Section: Transforming Nps and Clusters To Single Atomsmentioning

confidence: 99%

Recent Progress in Single‐Atom Catalysts for Photocatalytic Water Splitting

Zhang

Guan

2020

Solar RRL

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Photocatalytic water splitting can realize a direct conversion from solar energy into green hydrogen energy, which is conducive to effectively mitigate energy crisis and environmental issues. Single‐atom catalysts (SACs) have shown great potential in photocatalytic hydrogen evolution, with unique geometric and electronic structures that help to boost mass and charge transfer during photocatalytic processes. Herein, recent advances of SACs in photocatalytic water splitting are focused upon. To decrease aggregation and realize sufficient utilization of metal atoms, different synthesis strategies for SACs are documented. For photocatalytic hydrogen evolution, the catalytic performances, active sites, and structure–property relationships of SACs including Al, Co, Ni, Pd, Ag, and Pt single sites are highlighted. The existing challenges and future directions of SACs in photocatalytic water splitting are provided.

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“…The agglomeration of metal single atom can be avoided from the perspective of kinetics and thermodynamics by this method, which supplements the traditional nucleation theory and provides a new idea for the synthesis of various metal single atoms. Subsequently, combining this method with photoreduction, atomic‐level dispersed Pt catalyst can be prepared in ethanol solution for efficient hydrogen evolution reaction . The effects of temperature on the nuclear barrier of Pt single atom are analyzed by first‐principles molecular dynamics method combined with constrained minimization simulation technology.…”

Section: Controllable Synthesis Of Nonprecious Metal Sa‐npc Catalystsmentioning

confidence: 99%

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

et al. 2019

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Nonprecious metal single‐atom materials have attracted extensive attention in the field of electrocatalysis due to their low cost, high reactivity, high selectivity, and high atomic utilization. However, the high surface energy of a single atom causes agglomeration during preparation and catalytic measurement, resulting in damage to the catalytic sites. The strong interaction between substrate and monoatoms is the key factor to prevent the aggregation of individual metal atoms, and the geometry and electronic structure of the catalysts can be adjusted to optimize the catalytic activity. Due to the hierarchically pores, high specific surface area, and defect effect, nitrogen‐doped porous carbon (NPC) has been widely studied as an ideal nonprecious metal single‐atom support, which synergistically enhance the electrocatalytic performance toward oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction with non‐noble metal single atoms. This review summarizes the controllable synthesis, characterization, theoretical calculation, and application of M (M = Co, Fe, Ni, Cu, Zn, Mo, etc.) single atoms on nitrogen‐doped porous carbon. Finally, the future development and challenges of nitrogen‐doped porous carbon supported nonprecious metal single‐atom electrocatalysts for practical commercialization are concluded.

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Ultralow-temperature photochemical synthesis of atomically dispersed Pt catalysts for the hydrogen evolution reaction

Abstract: Atomically dispersed Pt is prepared by photochemical synthesis at a record-low temperature of −60 °C, which exhibits ultrahigh catalytic activity.

Cited by 89 publications

References 44 publications

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Recent Progress in Single‐Atom Catalysts for Photocatalytic Water Splitting

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

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