10 Search Results

Electrochemical reduction of carbon dioxide to organic chemicals provides a value-added route for mitigating greenhouse gas emissions. Here, we report a family of carbon-supported Sn electrocatalysts with the tin size varying from single atom, ultrasmall clusters to nanocrystallites. High single-product Faradaic efficiency (FE) and low onset potential of CO₂ conversion to acetate (FE = 90% @ –0.6 V), ethanol (FE = 92% @ –0.4 V), and formate (FE = 91% @ –0.6 V) were achieved over the catalysts of different active site dimensions. The CO₂ conversion mechanism behind these highly selective, size-modulated p-block element catalysts was elucidated by structural characterizationmore » and computational modeling, together with kinetic isotope effect investigation.« less

In this study, highly efficient and low-cost oxygen reduction reaction (ORR) catalyst is essential to improve the cost competitiveness of the proton-exchange membrane fuel cells (PEMFCs). One potential approach of cost reduction is to apply low loading Pt over a catalytically active support made of platinum metal group free (PGM-free) material to compensate the overall ORR activity through synergistic catalysis between Pt and PGM-free support. In this report, we investigated a series of catalysts prepared by adding low-loading Pt over ORR active support prepared through thermally activated Co/Zn methyl-imidazolate framework (Co/Zn-ZIF) at various Co/Zn ratios. Catalytic activity measurement and structuralmore » characterization were performed in an attempt to gain better understanding of certain structural factors that could influence the catalytic performance.« less

Discovery of earth-abundant electrocatalysts to replace iridium for the oxygen evolution reaction (OER) in a proton exchange membrane water electrolyzer (PEMWE) represents a critical step in reducing the cost for green hydrogen production. Here we report a nanofibrous cobalt spinel catalyst codoped with lanthanum (La) and manganese (Mn) prepared from a zeolitic imidazolate framework embedded in electrospun polymer fiber. The catalyst demonstrated a low overpotential of 353 millivolts at 10 milliamperes per square centimeter and a low degradation for OER over 360 hours in acidic electrolyte. A PEMWE containing this catalyst at the anode demonstrated a current density of 2000more » milliamperes per square centimeter at 2.47 volts (Nafion 115 membrane) or 4000 milliamperes per square centimeter at 3.00 volts (Nafion 212 membrane) and low degradation in an accelerated stress test.« less

Atomically dispersed Cu catalyst was designed for highly efficient hydroxylation of aryl iodides under mild conditions.

Doping Li with Ag or Al effectively modulate its inherent chemical activity and enables very stable Li metal batteries.

Bimetallic catalysts often outperform their monometallic counterparts due to the synergistic effect. Here we reported that the Ni/Ga co-functionalized HZSM-5 catalyst, specifically with Ni₁/Ga₁ stoichiometric ratio, shows significantly improved selectivity (above 80 %) and stability than the Ni/HZSM-5 catalyst and higher activity (with identical selectivity) than the Ga/HZSM-5 catalyst in ethane aromatization. According to the transient experiment, the Ga and Ni₁Ga₁/HZSM-5 catalysts show an induction period of a few minutes. However, for Ni/HZSM-5 and Ni₁Ga_1/3/HZSM-5, the induction period increased to >10 min and >30 min, respectively, where up to 100 % of ethane was converted into methane and coke throughmore » cracking/hydrogenolysis. Furthermore, based on the generalized power-law equation model, a modified model for deactivation kinetic was proposed. Consequently, the influence of the metal function on the kinetic parameters was discussed. We anticipate the formation of Ni₃Ga intermetallic alloy and its synergy with the exchanged Ga^δ+ to be responsible for optimal BTX formation.« less

Single-atom catalysts have emerged as a new frontier in catalysis science. However, their applications are still limited to small molecule activations in the gas phase, the classic organic transformations catalyzed by single-atom catalysts are still rare. Here, we report the use of a single-atom Pd catalyst for the classic Suzuki–Miyaura carbon–carbon coupling reaction under phosphine-free and open-air conditions at room temperature. The single-atom Pd catalyst is prepared through anchoring Pd on bimetal oxides (Pd-ZnO-ZrO₂). The significant synergetic effect of ZnO and ZrO₂ is observed. The catalyst exhibits high activity and tolerance of a wide scope of substrates. Characterization demonstrates thatmore » Pd single atoms are coordinated with two oxygen atoms in Pd-ZnO-ZrO₂ catalyst. The catalyst can be fabricated on a multi-gram scale using a simple in situ co-precipitation method, which endows this catalytic system with great potential in practical applications.« less

Direct electrochemical conversion of CO₂ to ethanol offers a promising strategy of lowering CO₂ emission while storing energy from renewable electricity. However, current electrocatalysts offer only limited selectivity toward ethanol. Here we report a copper catalyst synthesized by a unique Cu-Li amalgm method over a commercial carbon support that achieved Faradaic efficiency (FE) higher than 91% at -0.7 V (RHE) and the active potential as low as -0.4 V (RHE) during direct electrocatalytic CO₂-to-ethanol conversion. The catalyst also demonstrated stability over an extended period of operation. A strong correlation between the catalytic selectivity and the initial Cu atoms dispersion wasmore » found and Operando X-ray absorption spectroscopy identified a dynamic and reversible transformation from atomically dispersed copper atoms to Cu_n (n = 3 and 4) under the electrochemical reaction. Frist-principles calculations further elucidate the possible catalytic mechanism of CO₂ reduction over Cu_n.« less

The low-cost hydrogen production from water electrolysis is crucial to the deployment of sustainable hydrogen economy but is currently constrained by the lack of active and robust electrocatalysts from earth-abundant materials. We describe here an unconventional heterostructure composed of strongly coupled Ni-deficient LixNiO nanoclusters and polycrystalline Ni nanocrystals and its exceptional activities toward the hydrogen evolution reaction (HER) in aqueous electrolytes. Furthermore, the presence of lattice oxygen species with strong Brønsted basicity is a significant feature in such heterostructure, which spontaneously split water molecules for accelerated Volmer H-OH dissociation in neutral and alkaline HER. In combination with the intimate Li_xNiOmore » and Ni interfacial junctions that generate localized hotspots for promoted hydride coupling and hydrogen desorption, the catalysts produce hydrogen at a current density of 10 mA cm^-2 under overpotentials of only 20, 50, and 36 mV in acidic, neutral, and alkaline electrolytes, respectively, making them among the most active Pt-free catalysts developed thus far. In addition, such heterostructures also exhibited superior activity toward the hydrogen oxidation reaction in alkaline electrolytes.« less

We report an amorphous boron nanorod anode material for lithium-ion batteries prepared through smelting non-toxic boron oxide in liquid lithium.