Electrochemical reduction of carbon dioxide with renewable energy is a sustainable way producing carbon-neutral fuels. However, developing active, selective and stable electrocatalysts challenging entails material structure design tailoring across range length scales. Here we report cobalt-phthalocyanine-based high-performance electrocatalyst developed combined nanoscale molecular approach. On the nanoscale, cobalt phthalocyanine (CoPc) molecules are uniformly anchored on nanotubes to afford...

Exploration of heterogeneous molecular catalysts combining the atomic-level tunability structures and practical handling advantages represents an attractive approach to developing high-performance for important challenging chemical reactions such as electrochemical carbon dioxide reduction which holds promise converting emissions back fuels utilizing renewable energy. Thus, far, efficient selective electroreduction CO2 deeply reduced products hydrocarbons remains a big challenge. Here, we...

Chemistry at the cathode/electrolyte interface plays an important role for lithium-sulfur batteries in which stable cycling of sulfur cathode requires confinement lithium polysulfide intermediates and their fast electrochemical conversion on electrode surface. While many materials have been found to be effective confining polysulfides, underlying chemical interactions remain poorly understood. We report a new general polysulfide-binding mechanism enabled by surface oxidation layers...

Exploring materials with regulated local structures and understanding how the atomic motifs govern reactivity durability of catalysts are a critical challenge for designing advanced catalysts. Herein we report tuning structure nickel-iron layered double hydroxides (NiFe-LDHs) by partially substituting Ni2+ Fe2+ to introduce Fe-O-Fe moieties. These -containing NiFe-LDHs exhibit enhanced oxygen evolution reaction (OER) activity an ultralow overpotential 195 mV at current density 10 mA cm-2 ,...

Developing earth‐abundant, active, and stable electrocatalysts for water splitting is a vital but challenging step realizing efficient conversion storage of sustainable energy. Here, multiscale structure‐engineering approach to construct iron (Fe) doped cobalt monophosphide (CoP) hybrids electrocatalysis reported. A two‐step method developed synthesize CoP nanosheets with uniform Fe doping hybridization carbon nanotubes (CNTs). The nanostructuring, doping, CNT afford comparable Pt/C hydrogen...

The local pH variation near the surface of CO2 reduction electrodes is important but hard to study. We develop a continuous-flow Raman electrochemical cell that enables first experimental study gas diffusion electrode under reaction conditions. At zero current, chemically reacts with 1 M KOH electrolyte at interface form HCO3- and CO32-. on cathode 7.2, concentration profile extends distance 120 μm into electrolyte, which verifies nominal overpotential from using alkaline originates Nernst...

Stable-cycling Li metal anode is realized with a MOF layer regulating Li-ion transport and deposition<italic>via</italic>chemical interactions.

A versatile and straightforward room-temperature strategy is demonstrated to synthesize boundary defect-rich ultrathin transition metal hydroxide nanosheet networks by in situ etching of a cobalt metal–organic framework (Co-MOF, ZIF-L-Co). The resultant Co(OH)2 (D-U-Co(OH)2) nanoarray one the most active monometal-based oxygen evolution catalysts date. Its activity 3–4 times higher than that commercial RuO2 superior reported exfoliated bimetallic catalysts. Co-MOF can also be grown on...

NiFe-layered double hydroxide (LDH) is thought of as a promising bifunctional water-splitting catalyst, owing to its excellent performances for alkaline oxygen evolution reactions (OERs). However, it shows extremely poor activity toward hydrogen (HERs) due the weak adsorption. We demonstrated that integration Rh species and NiFe-LDH can dramatically improve HER kinetics without sacrificing OER performance. The were initially integrated into oxidized dopants metallic clusters (< 1 nm). In M...

Studying the restructuring behavior of doped catalyst materials under electrochemical reaction conditions is important for understanding structure–property relationships and developing design principles better catalysts. As a well-known both cathode (H2 evolution reaction, HER) anode (O2 OER) reactions water electrolysis, CoP can be made even more active by cationic or anionic substitution. However, dependence catalytic reactivity on substitutional doping has not been sufficiently understood...

We report the design, synthesis, and implemention in semiconducting polymers of a novel head-to-head linkage containing TRTOR (3-alkyl-3′-alkoxy-2,2′-bithiophene) donor subunit having single strategically optimized, planarizing noncovalent S···O interaction. Diverse complementary thermal, optical, electrochemical, X-ray scattering, electrical, photovoltaic, electron microscopic characterization techniques are applied to establish structure–property correlations TRTOR-based polymer series. In...

Black phosphorus (BP) has recently attracted significant attention due to its exceptional physical properties. Currently, high-quality few-layer and thin-film BP are produced primarily by mechanical exfoliation, limiting their potential in future applications. Here, the synthesis of highly crystalline on 5 mm sapphire substrates conversion from red black at 700 °C 1.5 GPa is demonstrated. The synthesized ≈50 nm thick thin films polycrystalline with a crystal domain size ranging 40 70 µm...

The promise and challenge of electrochemical mitigation CO2 calls for innovations on both catalyst reactor levels. In this work, enabled by our high-performance earth-abundant electroreduction materials, we developed alkaline microflow electrolytic cells energy-efficient, selective, fast, durable conversion to CO HCOO–. With a cobalt phthalocyanine-based cathode catalyst, the CO-selective cell starts operate at 0.26 V overpotential reaches Faradaic efficiency 94% partial current density 31...

Cu is a well-known electrocatalyst for reducing CO2 to various products. However, unmodified exhibits poor selectivity and activity formate production. Our in situ Raman spectroscopy study detects HCOO* intermediates on the surface under electroreduction reaction conditions confirms their reductive desorption being rate-limiting step of producing formate. We further show that cetyltrimethylammonium bromide (CTAB) can dramatically improve catalysis via competitive adsorption facilitate...

One major challenge to the electrochemical conversion of CO2 useful fuels and chemical products is lack efficient catalysts that can selectively direct reaction one desirable product avoid other possible side products. Making use strong metal/oxide interactions has recently been demonstrated be effective in enhancing electrocatalysis liquid phase. Here, we report first systematic studies on composition-dependent influences electrocatalytic reduction, utilizing Cu/SnOx heterostructured...

Transition-metal phosphosulfides represent an emerging category of earth-abundant electrocatalyst materials, and some metal have been shown to outperform the corresponding sulfides phosphides. To fully realize potential benefit energy storage conversion, it is necessary study chemistry unknown phosphosulfide materials. In this article, we report on materials iron phosphosulfides. We systematically investigate synthesis, solid state chemistry, surface structures, electrocatalytic properties...

Abstract Exploring materials with regulated local structures and understanding how the atomic motifs govern reactivity durability of catalysts are a critical challenge for designing advanced catalysts. Herein we report tuning structure nickel–iron layered double hydroxides (NiFe‐LDHs) by partially substituting Ni 2+ Fe to introduce Fe‐O‐Fe moieties. These ‐containing NiFe‐LDHs exhibit enhanced oxygen evolution reaction (OER) activity an ultralow overpotential 195 mV at current density 10 mA...

Significance The promise of lithium–sulfur batteries for future electric transportation and stationary energy storage is being limited by their poor cycling stability. Previous approaches to improvement often involve incorporating additional components with significant dead weight or volume in battery structures. We develop an ultrathin functionalized dendrimer–graphene oxide composite film which can be applied virtually any sulfur cathode alleviate capacity fading over without compromising...

Probing and understanding surface restructuring-induced electrocatalytic reactivity is an essential but challenging step toward rational prediction of properties design high-performance catalysts. Cobalt phosphide (CoP) nanoparticles are state-of-the-art electrocatalysts for both the hydrogen evolution reaction (HER) oxygen (OER). However, structure–reactivity correlations not straightforward because will restructure under working conditions. Employing a protective sample transfer procedure,...

Understanding how remarkable properties of materials emerge from complex interactions their constituents and designing advanced material structures to render desired are grand challenges. Metal–oxide frequently utilized improve catalytic but often limited situations where only one component is facilitated by the other. In this work, we demonstrate highly cooperative win-win metal–oxide that enable unprecedented functionalities for electrochemical CO2 reduction reactions. a single SnOx/Ag...

Strong interactions between two different types of metal nanoparticles can dramatically change their electrocatalytic properties but are underexplored. Herein we show that with Au turn Cu, which by itself is neither selective nor active for electrochemical CO2 reduction to formate, into a much improved electrocatalyst the same reaction. Our Cu/Au catalyst produces formate in significant yield at −0.4 V vs reversible hydrogen electrode near-neutral electrolyte and achieves partial current...

Abstract Developing electrolytes compatible with efficient and reversible cycling of electrodes is critical to the success rechargeable Li metal batteries (LMBs). The Coulombic efficiencies cycle lives LMBs ethylene carbonate (EC), dimethyl carbonate, sulfite (ES), their combinations as electrolyte solvents show that in a binary‐solvent extent decomposition on electrode surface dependent solvent component dominates solvation sheath + . This knowledge led development an EC‐ES exhibiting high...

Cobalt phosphide (CoP) is one of the most promising earth-abundant replacements for noble metal catalysts hydrogen evolution reaction (HER). Critical to HER binding H atoms. While theoretical studies have computed preferred sites and energetics bound transition surfaces, direct experimental are scarce. Herein, we describe measurements stoichiometry thermochemistry CoP. We studied both mesoscale CoP particles, exhibiting surfaces after an acidic pretreatment, colloidal nanoparticles....

Abstract Confining lithium polysulfide intermediates is one of the most effective ways to alleviate capacity fade sulfur‐cathode materials in lithium–sulfur (Li–S) batteries. To develop long‐cycle Li–S batteries, there an urgent need for material structures with binding capability and well‐defined surface sites; thereby improving cycling stability allowing study molecular‐level interactions. This challenge was addressed by introducing organometallic molecular compound, ferrocene, as a new...