A universal ligand mediated method for large scale synthesis of transition metal single atom catalysts

Yang, Hongzhou; Shang, Lu; Zhang, Qinghua; Shi, Run; Waterhouse, Geoffrey I. N.; Gu, Lin; Zhang, Tierui

doi:10.1038/s41467-019-12510-0

Cited by 551 publications

(405 citation statements)

References 34 publications

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“…SACs have shown excellent activity and selectivity in CO 2 RR for the conversion of CO 2 into value-added chemicals such as CO, formic acid, C 2 products, etc. (31,(139)(140)(141)(142)(143). Microenvironment engineering of SACs offers great opportunities for reducing the overpotential of CO 2 RR and improving the selectivity for the desired products.…”

Section: Co 2 Reduction Reactionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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Single-atom catalysts (SACs) have become the most attractive frontier research field in heterogeneous catalysis. Since the atomically dispersed metal atoms are commonly stabilized by ionic/covalent interactions with neighboring atoms, the geometric and electronic structures of SACs depend greatly on their microenvironment, which, in turn, determine the performances in catalytic processes. In this review, we will focus on the recently developed strategies of SAC synthesis, with attention on the microenvironment modulation of single-atom active sites of SACs. Furthermore, experimental and computational advances in understanding such microenvironment in association to the catalytic activity and mechanisms are summarized and exemplified in the electrochemical applications, including the water electrolysis and O2/CO2/N2 reduction reactions. Last, by highlighting the prospects and challenges for microenvironment engineering of SACs, we wish to shed some light on the further development of SACs for electrochemical energy conversion.

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Section: Co 2 Reduction Reactionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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“…Concerning the synthesis of SACs, areas for improvement include the development of strategies to achieve ultra-high loadings and to precisely control the speciation and nuclearity of atomically-dispersed species, as well as a greater focus on scalable routes to accelerate commercialization (Fig. 1, L14) 20 . Tool development needs to focus on resolving the local environment with increasing precision, quantifying the real dispersion of SACs -as minority element centers may not be located on the external surface of host materials -and the separation between neighboring sites.…”

Section: Frontiers In the Designmentioning

confidence: 99%

Single atom catalysis: a decade of stunning progress and the promise for a bright future

2020

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Controlling the hybridization of single atoms in suitable host materials opens unique opportunities for catalyst design, but equally faces many challenges. Here, we highlight emerging directions from the last, highly productive, decade in single-atom catalysis and identify frontiers for future research. Origins and evolution of single-atom catalysis The isolation of elements as atoms in chemically-distinct substances played fundamental catalytic roles, for example, in metalloenzymes, organometallic complexes, and open framework structures, long before this concept was extended to widely applied heterogeneous catalysts based on supported metals. In pioneering early work, Flytzani-Stephanopoulos et al. provided convincing evidence that ionic gold or platinum species strongly associated with the surface of ceria, and not the metal nanoparticles, were responsible for the activity observed in the water-gas shift reaction (Fig. 1, L1) 1. Subsequently, Bashyam and Zelenay proposed that oxidized cobalt and iron species coordinated to nitrogen and oxygen in functionalized carbons deliver high performance in the electrochemical oxygen reduction reaction (Fig. 1, L2) 2. After years of speculation about the catalytic role of single atoms of this group of elements, advances in experimental techniques made it possible to confirm the exclusive presence of isolated centers. In their landmark paper, Zhang et al. confirmed the high efficiency of platinum atoms supported on iron oxide for CO oxidation, introducing a new paradigm in heterogeneous catalysis (Fig. 1, L3) 3. The first catalytic applications of single-atom alloys based on metal hosts followed shortly after (Fig. 1, L5) 4. In just a decade, the topic of single-atom catalysis has become a highly transversal field of contemporary chemical research. Early researchers quickly recognized the potential cost benefits of using atomically-dispersed species for precious metals, and improving the utilization became a central driver in the topic. As the area developed, the motivation also evolved. Comparative studies revealed that the strategy of using SACs does not apply to all applications and depends on the reaction requirements 5. Another strength is the higher uniformity of potential active sites in heterogeneous catalysts based on single atoms compared to nanoparticles. The well-defined nature is attractive for both defining structure-function relationships and computational modeling. Furthermore, the close structural resemblance to molecular complexes provides a bridge between homogeneous and heterogeneous catalysis. On the 10-year journey since the consolidation of the topic, single-atom catalysis has crossed the periodic table. The diversity of host materials has also expanded. While metal oxides were initially most widely studied, tailored carbons have superseded all other types in the last years.

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“…The Ni SACs selectively reduced CO 2 to CO with a TOF of 11.7 s −1 at −0.55 V. Notably, Zhang's group developed a universal strategy for fabricating transition metal single‐atom catalysts (e.g., Cr, Mn, Fe, Co, Ni, Cu, Zn, Ru, Pt or their combinations) with high metal mass loadings in large quantities (>1 kg scale). [ 96 ] The mass loadings could reach up to 1.8 wt% for all the metals, and the highest loading of 5.32 wt% was achieved for single Ni atoms. The developed strategy is believed capable of paving the progress of synthesizing SACs in large scale.…”

Section: Modifying the Nanostructured Electrocatalysts At Atomic Scalmentioning

confidence: 99%

Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO₂ Reduction

Liu

Zhu

et al. 2020

Adv Funct Materials

116

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Electrochemical reduction of CO 2 into value-added chemicals provides a promising approach to mitigate climate change caused by CO 2 from excess consumption of fossil fuels. As the CO 2 molecule is chemically inert and the reaction kinetics is sluggish, efficient electrocatalysts are thus highly required for promoting the conversion of CO 2 . With great efforts devoted to improving the catalytic performance, the development of electrocatalysts for CO 2 reduction has gone from bulk metals with poor control to nanostructures with atomic precision. Nanostructured electrocatalysts with atomic precision are believed to be capable of combining the advantages of heterogeneous and homogenous catalysts. In this review, the recent advances in designing nanostructured electrocatalysts at the atomic level for boosting the catalytic performance toward CO 2 reduction and revealing the structure-property relationship are summarized. The challenges and opportunities in the near future are also proposed for paving the development of electrocatalytic CO 2 reduction.half reactions and equilibrium potentials (versus reversible hydrogen electrode (RHE)) are listed as Reaction (1) to (6): [7] CO 2H 2e HCOOH 0.12 V Adv. Funct.

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A universal ligand mediated method for large scale synthesis of transition metal single atom catalysts

Cited by 551 publications

References 34 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Single atom catalysis: a decade of stunning progress and the promise for a bright future

Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO₂ Reduction

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A universal ligand mediated method for large scale synthesis of transition metal single atom catalysts

Cited by 551 publications

References 34 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Single atom catalysis: a decade of stunning progress and the promise for a bright future

Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO2 Reduction

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Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO₂ Reduction