Utilizing reconstruction achieves ultrastable water electrolysis.

The dissolution of active atoms under operating potential will lead to a decline in their oxygen evolution reaction (OER) performance, thus preventing the current highly active catalysts from being practically applicable in industrial water electrolysis. Here, we propose a sequential leaching strategy to utilize the dynamic restructuring and enhance the chemical bond strength for highly active and stable OER. Modeling on nickel-iron sulfides (NiFe-S), we introduced and utilized foreign Mo dopant preleaching as the sacrificial agent to alleviate the oxidation corrosion of partial M─S bonds.

Directional Reconstruction to Highly Active Tandem Sites for Superior Acidic CO Electroreduction.

Acidic CO electroreduction (COR) to multi-carbon (C) chemicals advance the carbon neutrality in the manner of high carbon utilization efficiency; however, it suffers from low selectivity. Designing tandem catalysts is the most promising remedy, yet achieving highly active tandem sites remains an immense challenge due to the potentiodynamic structural evolution. Here self-reducing ion (e.

Strain-induced charge delocalization achieves ultralow exciton binding energy toward efficient photocatalysis.

The exciton effect is commonly observed in photocatalysts, where substantial exciton binding energy ( ) significantly hampers the efficient generation of photo-excited electron-hole pairs, thereby severely constraining photocatalysis. Herein, we propose a strategy to reduce through strain-induced charge delocalization. Taking TaO as a prototype, tensile strain was introduced by engineering a crystalline/amorphous interface, weakening the interaction between Ta 5d and O 2p orbitals, thus endowing a delocalized charge transport and significantly lowering .

Operando-reconstructed polyatomic ion layers boost the activity and stability of industrial current-density water splitting.

Metal-organic frameworks have garnered attention as highly efficient pre-electrocatalysts for the oxygen evolution reaction (OER). Current structure-activity relationships primarily rely on the assumption that the complete dissolution of organic ligands occurs during electrocatalysis. Herein, modeling based on NiFe Prussian blue analogs (NiFe-PBAs) show that cyanide ligands leach from the matrix and subsequently oxidize to corresponding inorganic ions (ammonium and carbonate) that re-adsorb onto the surface of NiFe OOH during the OER process.

Reconstructing Hydrogen-Bond Network for Efficient Acidic Oxygen Evolution.

Developing highly active oxygen evolution reaction (OER) catalysts in acidic conditions is a pressing demand for proton-exchange membrane water electrolysis. Manipulating proton character at the electrified interface, as the crux of all proton-coupled electrochemical reactions, is highly desirable but elusive. Herein we present a promising protocol, which reconstructs a connected hydrogen-bond network between the catalyst-electrolyte interface by coupling hydrophilic units to boost acidic OER activity.

Sequential *CO management via controlling in situ reconstruction for efficient industrial-current-density CO-to-C electroreduction.

Sequentially managing the coverage and dimerization of *CO on the Cu catalysts is desirable for industrial-current-density CO reduction (COR) to C, which required the multiscale design of the surface atom/architecture. However, the oriented design is colossally difficult and even no longer valid due to unpredictable reconstruction. Here, we leverage the synchronous leaching of ligand molecules to manipulate the seeding-growth process during COR reconstruction and construct Cu arrays with favorable (100) facets.

Scalable synthesis of Cu clusters for remarkable selectivity control of intermediates in consecutive hydrogenation.

Subnanometric Cu clusters that contain only a small number of atoms exhibit unique and, often, unexpected catalytic behaviors compared with Cu nanoparticles and single atoms. However, due to the high mobility of Cu species, scalable synthesis of stable Cu clusters is still a major challenge. Herein, we report a facile and practical approach for scalable synthesis of stable supported Cu cluster catalysts.

Palladium catalyzed radical relay for the oxidative cross-coupling of quinolines.

Traditional approaches for transition-metal catalyzed oxidative cross-coupling reactions rely on sp-hybridized starting materials, such as aryl halides, and more specifically, homogeneous catalysts. We report a heterogeneous Pd-catalyzed radical relay method for the conversion of a heteroarene C(sp)-H bond into ethers. Pd nanoparticles are supported on an ordered mesoporous composite which, when compared with microporous activated carbons, greatly increases the Pd d charge because of their strong interaction with N-doped anatase nanocrystals.

Active and conductive layer stacked superlattices for highly selective CO electroreduction.

Metal oxides are archetypal CO reduction reaction electrocatalysts, yet inevitable self-reduction will enhance competitive hydrogen evolution and lower the CO electroreduction selectivity. Herein, we propose a tangible superlattice model of alternating metal oxides and selenide sublayers in which electrons are rapidly exported through the conductive metal selenide layer to protect the active oxide layer from self-reduction. Taking BiCuSeO superlattices as a proof-of-concept, a comprehensive characterization reveals that the active [BiO] sublayers retain oxidation states rather than their self-reduced Bi metal during CO electroreduction because of the rapid electron transfer through the conductive [CuSe] sublayer.

Tandem Catalysis for Selective Oxidation of Methane to Oxygenates Using Oxygen over PdCu/Zeolite.

Selective oxidation of methane to oxygenates with O under mild conditions remains a great challenge. Here we report a ZSM-5 (Z-5) supported PdCu bimetallic catalyst (PdCu/Z-5) for methane conversion to oxygenates by reacting with O in the presence of H at low temperature (120 °C). Benefiting from the co-existence of PdO nanoparticles and Cu single atoms via tandem catalysis, the PdCu/Z-5 catalyst exhibited a high oxygenates yield of 1178 mmol g  h (mmol of oxygenates per gram Pd per hour) and at the same time high oxygenates selectivity of up to 95 %.

In Situ Halogen-Ion Leaching Regulates Multiple Sites on Tandem Catalysts for Efficient CO Electroreduction to C Products.

Tandem catalysts can divide the reaction into distinct steps by local multiple sites and thus are attractive to trigger CO RR to C products. However, the evolution of catalysts generally exists during CO RR, thus a closer investigation of the reconstitution, interplay, and active origin of dual components in tandem catalysts is warranted. Here, taking AgI-CuO as a conceptual tandem catalyst, we uncovered the interaction of two phases during the electrochemical reconstruction.

In Situ Phase Separation into Coupled Interfaces for Promoting CO Electroreduction to Formate over a Wide Potential Window.

Bimetallic sulfides are expected to realize efficient CO electroreduction into formate over a wide potential window, however, they will undergo in situ structural evolution under the reaction conditions. Therefore, clarifying the structural evolution process, the real active site and the catalytic mechanism is significant. Here, taking Cu SnS as an example, we unveiled that Cu SnS occurred self-adapted phase separation toward forming the stable SnO @CuS and SnO @Cu O heterojunction during the electrochemical process.

Single WTe Sheet-Based Electrocatalytic Microdevice for Directly Detecting Enhanced Activity of Doped Electronegative Anions.

The high electrical conductivity of 1T'-WTe deserves particular attention and may show a high potential for hydrogen evolution reaction (HER) catalysis. However, the actual activity certainly does not match expectations, and the inferior HER activity is actually still ambiguous at the atomic level. Unraveling the underlying HER behaviors of 1T'-WTe will give rise to a new family of HER catalysts.

Cu single-atoms embedded in porous carbon nitride for selective oxidation of methane to oxygenates.

Cu single atoms embedded in the CN (Cu-SAs/CN) matrix exhibited high activity with 95% oxygenate selectivity for the direct conversion of methane at ambient temperature. The presence of abundant anchoring sites in CN led to highly dispersed Cu-N moieties, which were suggested to be the underlying active sites for methane conversion.

Vacancy-Rich Ni(OH) Drives the Electrooxidation of Amino C-N Bonds to Nitrile C≡N Bonds.

Electrochemical synthesis based on electrons as reagents provides a broad prospect for commodity chemical manufacturing. A direct one-step route for the electrooxidation of amino C-N bonds to nitrile C≡N bonds offers an alternative pathway for nitrile production. However, this route has not been fully explored with respect to either the chemical bond reforming process or the performance optimization.

Unleash electron transfer in C-H functionalization by mesoporous carbon-supported palladium interstitial catalysts.

The functionalization of otherwise unreactive C-H bonds adds a new dimension to synthetic chemistry, yielding useful molecules for a range of applications. Arylation has emerged as an increasingly viable strategy for functionalization of heteroarenes which constitute an important class of structural moieties for organic materials. However, direct bisarylation of heteroarenes to enable aryl-heteroaryl-aryl bond formation remains a formidable challenge, due to the strong coordination between heteroatom of N or S and transitional metals.

Subnanometer Bimetallic Platinum-Zinc Clusters in Zeolites for Propane Dehydrogenation.

Propane dehydrogenation (PDH) has great potential to meet the increasing global demand for propylene, but the widely used Pt-based catalysts usually suffer from short-term stability and unsatisfactory propylene selectivity. Herein, we develop a ligand-protected direct hydrogen reduction method for encapsulating subnanometer bimetallic Pt-Zn clusters inside silicalite-1 (S-1) zeolite. The introduction of Zn species significantly improved the stability of the Pt clusters and gave a superhigh propylene selectivity of 99.

In situ XAFS study on the formation process of cobalt carbide by Fischer-Tropsch reaction.

Fischer-Tropsch (F-T) synthesis is an effective approach to convert the syngas of H and CO into lower olefin and other valuable products for the chemical industry. Cobalt carbide (CoC), which was regarded as the sign of activity loss in the past, has recently been recognized as a highly-active phase for F-T synthesis. However, systematic study on the formation process of CoC by F-T reaction is still lacking.

An Isolated Zinc-Cobalt Atomic Pair for Highly Active and Durable Oxygen Reduction.

A competitive complexation strategy has been developed to construct a novel electrocatalyst with Zn-Co atomic pairs coordinated on N doped carbon support (Zn/CoN-C). Such architecture offers enhanced binding ability of O , significantly elongates the O-O length (from 1.23 Å to 1.

Uniform Pt quantum dots-decorated porous g-CN nanosheets for efficient separation of electron-hole and enhanced solar-driven photocatalytic performance.

Uniform Pt quantum dots-decorated porous g-CN nanosheets (Pt/CN) are fabricated by a facile impregnation-ultrasonic-calcination method, using melamine as precursor. The as-prepared samples are evidently investigated by X-ray diffraction, UV-vis diffuse reflection spectra, N adsorption, transmission electron microscope, surface photovoltage spectroscopy and photoluminescence. The deposited Pt quantum dots with particle size of ∼5 nm are decorated on the surface of porous g-CN nanosheets uniformly.

Iron Vacancies Induced Bifunctionality in Ultrathin Feroxyhyte Nanosheets for Overall Water Splitting.

Exploring of new catalyst activation principle holds a key to unlock catalytic powers of cheap and earth-abundant materials for large-scale applications. In this regard, the vacancy defects have been proven to be effective to initiate catalytic active sites and endow high electrocatalytic activities. However, such electrocatalytically active defects reported to date have been mostly formed by anion vacancies.

Heat treated carbon supported iron(ii)phthalocyanine oxygen reduction catalysts: elucidation of the structure-activity relationship using X-ray absorption spectroscopy.

This paper focuses on studying the influence of the heat treatment on the structure and activity of carbon supported Fe(ii)phthalocyanine (FePc/C) oxygen reduction reaction (ORR) catalysts under alkaline conditions. The FePc macrocycle was deposited onto ketjen black carbon and heated treated for 2 hours under inert atmosphere (Ar) at different temperatures (400, 500, 600, 700, 800, 900 and 1000 °C). The atomic structure of Fe in each sample has been determined by XAS and correlated to the activity and ORR mechanisms determined in electrochemical half cells and in a complete H/O anion exchange membrane fuel cells (AEM-FC).