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We report a simple route based upon seed‐mediated growth to the synthesis of Pd@AuxPd1−x (0.8≤x≤1) core–shell nanocubes. Benefiting from the well‐defined {100} facets and an optimal Au/Pd ratio for the surface, the nanocubes bearing a shell made of Au0.95Pd0.05 work as an efficient electrocatalyst toward H2O2 production, with high selectivity of 93–100 % in the low‐overpotential region of 0.4–0.7 V. When the Au0.95Pd0.05 alloy is confined to a shell of only three atomic layers in thickness, the electrocatalyst is able to maintain its surface structure and elemental composition, endowing continuous and stable production of H2O2 during oxygen reduction at a high rate of 1.62 mol g(Pd+Au)−1 h−1. This work demonstrates a versatile route to the rational development of active and durable electrocatalysts based upon alloy nanocrystals. [ABSTRACT FROM AUTHOR]

Forming an ultra‐thin, permeable encapsulation oxide‐support layer on a metal catalyst surface is considered an effective strategy for achieving a balance between high stability and high activity in heterogenous catalysts. The success of such a design relies not only on the thickness, ideally one to two atomic layers thick, but also on the morphology and chemistry of the encapsulation layer. Reliably identifying the presence and chemical nature of such a trace layer has been challenging. Electron energy‐loss spectroscopy (EELS) performed in a scanning transmission electron microscope (STEM), the primary technique utilized for such studies, is limited by a weak signal on overlayers when using conventional analysis methods, often leading to misinterpreted or missed information. Here, a robust, unsupervised machine learning data analysis method is developed to reveal trace encapsulation layers that are otherwise overlooked in STEM‐EELS datasets. This method provides a reliable tool for analyzing encapsulation of catalysts and is generally applicable to any spectroscopic analysis of materials and devices where revealing a trace signal and its spatial distribution is challenging. [ABSTRACT FROM AUTHOR]

The article titled "Back Cover: Significant Roles of Surface Hydrides in Enhancing the Performance of Cu/BaTiO2.8H0.2 Catalyst for CO2 Hydrogenation to Methanol" discusses the use of surface hydrides in improving the efficiency of a catalyst for converting CO2 to methanol. The cover picture depicts a BaTiO3 lattice with Cu nanoparticles representing the catalytic process. The researchers, led by Zili Wu, demonstrate that replacing lattice oxygen with hydrides enhances the catalyst's performance. The article provides valuable insights into the reaction mechanism and includes an operando study. [Extracted from the article]

We report a facile synthesis of Ag@Pd core−shell icosahedral nanocrystals for the development of cost‐effective electrocatalysts toward formic acid oxidation. With 12.4 nm Ag icosahedra serving as seeds, Pd shells of controlled thicknesses in the range of 3.6–5.8 atomic layers are grown by adjusting the experimental parameters. When examined as catalysts toward formic acid oxidation, all the Ag@Pd nanocrystals exhibit enhanced mass activities relative to a commercial Pd/C catalyst, with the Ag@Pd4.2L nanocrystals showing enhanced mass activity that is almost twice that of a commercial Pd/C. The chronoamperometry measurements indicate that all the Ag@Pd/C catalysts are more robust than the Pd/C, with the catalyst based on Ag@Pd4.2L nanocrystals showing a mass activity greater than that of the pristine Pd/C after holding in a mixture of HCOOH and HClO4 at 0.75 V for 1,000 s. We believe that the strategy demonstrated here can also be extended to the development of other types of advanced electrocatalysts. [ABSTRACT FROM AUTHOR]

The development of dual catalysts with high efficiency toward oxygen reduction and evolution reactions (ORR and OER) in acidic media is a significant challenge. Here an active and durable dual catalyst based upon cubic Pt39Ir10Pd11 nanocages with an average edge length of 12.3 nm, porous walls as thin as 1.0 nm, and well‐defined {100} facets is reported. The trimetallic nanocages perform better than all the reported dual catalysts in acidic media, with a low ORR‐OER overpotential gap of only 704 mV at a Pt‐Ir‐Pd loading of 16.8 µgPt+Ir+Pd cm−2geo. For ORR at 0.9 V, when benchmarked against the commercial Pt/C and Pt‐Pd nanocages, the trimetallic nanocages exhibit an enhanced mass activity of 0.52 A mg−1Pt+Ir+Pd (about four and two times as high as those of the Pt/C and Pt‐Pd nanocages) and much improved durability. For OER, the trimetallic nanocages show a remarkable mass activity of 0.20 A mg−1Pt+Ir at 1.53 V, which is 16.7 and 4.3 fold relative to those of the Pt/C and Pt‐Pd nanocages, respectively. These improvements can be ascribed to the highly open structure of the nanocages, and the possible electronic coupling between Ir and Pt atoms in the lattice. [ABSTRACT FROM AUTHOR]

Efficient electro‐oxidation of formic acid, methanol, and ethanol is challenging owing to the multiple chemical reaction steps required to accomplish full oxidation to CO2. Herein, a ternary CoPtAu nanoparticle catalyst system is reported in which Co and Pt form an intermetallic L10‐structure and Au segregates on the surface to alloy with Pt. The L10‐structure stabilizes Co and significantly enhances the catalysis of the PtAu surface towards electro‐oxidation of ethanol, methanol, and formic acid, with mass activities of 1.55 A/mgPt, 1.49 A/mgPt, and 11.97 A/mgPt, respectively in 0.1 m HClO4. The L10‐CoPtAu catalyst is also stable, with negligible degradation in mass activities and no obvious Co/Pt/Au composition changes after 10 000 potential cycles. The in situ surface‐enhanced infrared absorption spectroscopy study indicates that the ternary catalyst activates the C−C bond more efficiently for ethanol oxidation. [ABSTRACT FROM AUTHOR]

We have synthesized Pd icosahedra with uniform, controllable sizes in plug reactors separated by air. The oxygen contained in the air segments not only contributed to the generation of a reductant from diethylene glycol in situ, but also oxidized elemental Pd back to the ionic form by oxidative etching and thus slowed down the reduction kinetics. Compared to droplet reactors involving silicone oil or fluorocarbon, the use of air as a carrier phase could reduce the production cost by avoiding additional procedures for the separation of products from the oil. The average diameters of the Pd icosahedra could be readily controlled in the range of 12-20 nm. The Pd icosahedra were further employed as seeds for the production of Pd@Pt2-3L core-shell icosahedra, which could serve as a catalyst toward the oxygen reduction reaction with greatly enhanced activity. We believe that the plug reactors could be extended to other types of noble-metal nanocrystals for their scale-up production. [ABSTRACT FROM AUTHOR]

Machine Learning: Machine Learning Method Reveals Hidden Strong Metal-Support Interaction in Microscopy Datasets (Small Methods 5/2021) Catalysts, electron energy loss spectroscopy, encapsulation, machine learning, scanning transmission electron microscopy Keywords: catalysts; electron energy loss spectroscopy; encapsulation; machine learning; scanning transmission electron microscopy EN catalysts electron energy loss spectroscopy encapsulation machine learning scanning transmission electron microscopy 1 1 1 05/17/21 20210501 NES 210501 In article number 2100035, Ramakrishnan Kannan, Xiaoqing Pan, Miaofang Chi, and co-workers developed a robust, unsupervised machine learning data analysis method to reveal encapsulation of metal catalysts that are otherwise overlooked in microscopy datasets. [Extracted from the article]

• Improved syngas conversion to oxygenates over mixed Mo/Co carbide catalysts. • Catalysts form well mixed, amorphous carbidic and bimetallic nanoparticles. • Mo and Co reaction sites are in close contact at the catalyst surface. Recently metal carbide catalysts have attracted attention as alternatives to pure metals for the conversion of syngas to higher oxygenates, a process which could enable the sustainable production of fuels, polymers, and chemicals. Although Mo and Co carbides have both shown promise for higher oxygenate production, they have not achieved the requisite activity and selectivity for practical implementation. In this work we synthesize and characterize a binary Mo and Co carbide catalyst that exhibits improved activity and oxygenate selectivity relative to either pure metal carbide. We apply a combination of advanced electron microscopy and X-ray diffraction to show that the binary Mo/Co carbide catalyst forms uniformly mixed amorphous nanoparticles. Through in situ X-ray absorption spectroscopy studies, we determine that the structure of the mixed metal carbide catalyst under reaction conditions consists of both carbidic and bimetallic components. By testing the catalytic properties of a series of Mo/Co carbide catalysts prepared by different synthesis methods, we find that the Mo and Co sites must be in close contact to achieve improved syngas conversion to higher alcohols. Through in situ DRIFTS measurements, both Mo and Co atoms at the surface of the catalyst are identified as adsorption sites for reactive species. [ABSTRACT FROM AUTHOR]

Gold clusters, Au25 and Au144, after removal of their protecting thiolate ligands by thermal treatment are stabilized by heterostructured mesoporous CuO-mSiO2 and Co3O4-mSiO2 supports. [ABSTRACT FROM AUTHOR]

• A heterostructured catalyst based on high–entropy material was prepared. • Cu species in HEO dissolved into CeO 2 via an entropy-driven mechanochemical process. • The heterostructure was between high–entropy oxides and CeCuO x. • The heterostructured catalyst showed high-temperature stability for CO oxidation. Designing high-performance catalysts that can stabilize catalytic active sites against sintering to deactivation at temperature higher than 900 °C is significant but challenging. Here we report a new strategy to obtain a transition metal oxide catalyst with high temperature stability for CO oxidation. This is achieved through a synergistic interfacial interaction at the interface of a heterostructure between high–entropy oxides (HEO, high temperature stability) and CuCeO x (catalytic site). The catalytic site (CuCeO x) for CO oxidation is realized by dissolving an amount of Cu species in HEO into CeO 2 via an entropy–driven mechanochemical process. In situ XRD and HAADF–STEM have confirmed the high temperature stability of the heterostructure CuCeO x –HEO, which can remain its CO oxidation catalytic activity at elevated temperatures. It should be expected that this innovative will offer the potential to the synthesis of catalysts with high temperature stability in industry. [ABSTRACT FROM AUTHOR]