Catalysis by clusters with precise numbers of atoms

Tyo, Eric C.; Vajda, Štefan

doi:10.1038/nnano.2015.140

Cited by 635 publications

(512 citation statements)

References 113 publications

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“…Although Fe-, Co-and Ni-based oxides and derivatives are intensively studied as OER catalysts, the size dependence of electronic structure and catalytic reactivity suggests that the atomic metals within M-NHGFs could have different catalytic behaviour 47 . In addition, the catalytic properties of SACs can be tuned by a Co-Co Articles Nature Catalysis ligand-field effect, which differs depending on the identity of the metal centres and their interaction with the coordination configuration.…”

Section: Theoretical and Experimental Evaluation On Oer Activitymentioning

confidence: 99%

General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities

et al. 2018

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E fficient and cost-effective electrocatalysts play critical roles in energy conversion and storage [1][2][3] . Homogeneous and heterogeneous catalysts represent two parallel frontiers of electrocatalysts, each with their own merits and drawbacks 4,5 . Homogeneous catalysts are attractive for their highly uniform active sites, tunable coordination environment and maximized atom utilization efficiency, but are limited by their relatively poor stability and recyclability. Heterogeneous catalysts are appealing for their high durability, excellent recyclability, and easy immobilization and integration with electrodes, but usually have rather low atom utilization efficiency due to the limited surface sites accessible to reactants. To this end, considerable efforts have been devoted to developing nanoscale heterogeneous catalysts that can increase the exposed surface atoms 3 . However, the inhomogeneity in the distribution of particle sizes and facets poses a serious challenge for controlling active sites and fundamental mechanistic studies 6,7 . In contrast, homogeneous catalysts typically exhibit the well-defined atomic structure with tunable coordination environment that is essential for deciphering the catalytic reaction pathway and rational design of targeted catalysts with tailored catalytic properties 8 . Single-atom catalysts (SACs) with monodispersed single atoms supported on solid substrates are recently emerging as an exciting class of catalysts that combine the merits of both homogeneous and heterogeneous catalysts [9][10][11][12][13][14] . However, most SACs studied to date employ metal oxides (for example, TiO 2 , CeO 2 and FeO x ) as supporting substrates to prevent atom aggregation [15][16][17][18] , which cannot be readily applied in electrocatalytic applications due to their low electrical conductivity and/or poor stability in harsh liquid-phase electrolytes (for example, strong acid or base). Atomic transitionmetal-nitrogen moieties supported in carbon (M-N-Cs) represent a unique class of SACs with high electrical conductivity and superior (electro)chemical stability for electrocatalytic applications 19 . In particular, Fe-based M-N-Cs have been extensively studied as electrocatalysts towards the oxygen reduction reaction (ORR) with demonstrated activity and stability approaching those of commercial Pt/C catalysts 20,21 . In addition, as suggested by numerous theoretical studies, M-N-Cs are promising candidates for catalysing a wide range of electrochemical processes, such as hydrogen reduction/oxidation 22 , CO 2 /CO reduction 23 and N 2 reduction 24 . A significant advantage of SACs is that the well-defined single atomic site could allow precise understanding of the catalytic reaction pathway, and rational design of targeted catalysts with tailored activity (in a manner similar to homogeneous catalyst design). However, this perceived advantage has been investigated theoretically

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Section: Theoretical and Experimental Evaluation On Oer Activitymentioning

confidence: 99%

General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities

et al. 2018

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“…While significant strides towards atomically precise synthesis of metal NPs have been made in recent years, [12][13][14] the catalytic mechanisms operational at NP surfaces are not yet entirely understood. It is commonly accepted that clean/pristine NP surfaces are preferable in well-behaved catalysts.…”

Section: Introductionmentioning

confidence: 99%

Controllable Catalysis with Nanoparticles: Bimetallic Alloy Systems and Surface Adsorbates

2016

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Transition metal nanoparticles are privileged materials in catalysis due to their high specific surface areas and abundance of active catalytic sites. While many of these catalysts are quite useful, we are only beginning to understand the underlying catalytic mechanisms. Opening the "black box" of nanoparticle catalysis is essential to achieve the ultimate goal of catalysis by design. In this Perspective we highlight recent work addressing the topic of controlled catalysis with bimetallic alloy and "designer" adsorbate-stabilized metal nanoparticles.

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“…In addition to these unique features, the proposed NP synthesis method yields sub-5-nm singlet particles 27,31 , whose size can be tuned even down to that of atomic clusters (i.e., of the order of a few Å). 32 Particles in this size range not only provide an extremely large surface area for sufficiently high mass specific activity and diffusional deposition efficiency, but they also guarantee strong adhesion to fibers (given that agglomeration is avoided), thus minimizing their release. Since the NP synthesis method is fully compatible with commercial roll-to-roll textile production as illustrated in Figure 1, the nanofinishing process proposed here is amenable to upscaling.…”

Section: Introductionmentioning

confidence: 99%

Scalable and Environmentally Benign Process for Smart Textile Nanofinishing

Feng

Hontañón

Blanes

et al. 2016

ACS Appl. Mater. Interfaces

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A major challenge in nanotechnology is that of determining how to introduce green and sustainable principles when assembling individual nanoscale elements to create working devices.For instance, textile nanofinishing is restricted by the many constraints of traditional pad-drycure processes, such as the use of costly chemical procedures to produce nanoparticles (NPs), the high liquid and energy consumption, the production of harmful liquid waste, and multi-step batch operations. By integrating low-cost, scalable, and environmentally benign aerosol processes of the type proposed here into textile nanofinishing, these constraints can be circumvented while leading to a new class of fabrics. The proposed one-step textile nanofinishing process relies on the diffusional deposition of aerosol NPs onto textile fibers. As proof of this concept, we deposit Ag NPs onto a range of textiles and assess their antimicrobial properties for two strains of bacteria (i.e., Staphylococcus Aureus and Klebsiella Pneumoniae).The measurements show that the logarithmic reduction in bacterial count reaches ca. 5.5 (corresponding to a reduction efficiency of 99.96%) when the Ag loading is one order of magnitude less (10 ppm; i.e., 10 mg Ag NPs per kg of textile) than in the textiles treated by traditional wet-routes. The antimicrobial activity does not increase in proportion to the Ag content above 10 ppm as a consequence of a "saturation" effect. Such low loading for

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Catalysis by clusters with precise numbers of atoms

Cited by 635 publications

References 113 publications

General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities

General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities

Controllable Catalysis with Nanoparticles: Bimetallic Alloy Systems and Surface Adsorbates

Scalable and Environmentally Benign Process for Smart Textile Nanofinishing

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