Electrocatalytic Reduction of Carbon Dioxide to Methane on Single Transition Metal Atoms Supported on a Defective Boron Nitride Monolayer: First Principle Study

The electrochemical conversion of carbon dioxide (CO2) and water into useful multi‐electron transfer products, such as methanol (CH3OH) and methane (CH4), is a major challenge in facilitating a closed carbon cycle. Here, a systematic first principle study of the potential of single transition metal atoms (Sc to Zn, Mo, Rh, Ru, Pd, Ag, Pt, and Au) supported on experimentally available defective boron nitride monolayers with a boron monovacancy (TM/defective BN) to achieve highly efficient electrocatalytic CO2 reduction (ECR) to CH4 is carried out. Our computations reveal that Fe/defective BN, Co/defective BN, and Pt/defective BN nanosheets possess outstanding ECR activities with quite low (less negative) onset potentials of −0.52, −0.68, and −0.60 V, respectively. Given that Fe and Co are nonprecious metals, Fe/defective BN and Co/defective BN may provide cost‐effective electrocatalysts. The high ECR activities of these TM/defective BN catalyst systems stem from the moderate electrocatalysts’ affinities for C and O, which modulate the free energies of ECR intermediates in the reaction pathways. Moreover, it is found that Fe/defective BN and Pt/defective BN show high selectivity of ECR to CH4. This finding highlights a strategy to design highly active and selective single‐atom electrocatalysts for ECR to CH4.S.S. and H.A. acknowledge the financial support by the Australian Research Council under Discovery Project (DP170104853). This research was undertaken with the assistance of resources provided by the National Computing Infrastructure facility at the Australian National University, allocated through both the National Computational Merit Allocation Scheme supported by the Australian Government and the Australian Research Council grant LE120100181 (Enhanced merit-based access and support at the new NCI petascale supercomputing facility, 2012–2015)

Impact of surface defects on LaNiO3 perovskite electrocatalysts for the oxygen evolution reaction

Perovskite oxides are regarded as promising electrocatalysts for water splitting due to their cost-effectiveness, high efficiency and durability in the oxygen evolution reaction (OER). Despite these advantages, a fundamental understanding of how critical structural parameters of perovskite electrocatalysts influence their activity and stability is lacking. Here, we investigate the impact of structural defects on OER performance for representative LaNiO3 perovskite electrocatalysts. Hydrogen reduction of 700¿°C calcined LaNiO3 induces a high density of surface oxygen vacancies, and confers significantly enhanced OER activity and stability compared to unreduced LaNiO3; the former exhibit a low onset overpotential of 380 mV at 10 mA¿cm-2 and a small Tafel slope of 70.8 mV¿dec-1. Oxygen vacancy formation is accompanied by mixed Ni2+/Ni3+ valence states, which quantum-chemical DFT calculations reveal modify the perovskite electronic structure. Further, it reveals that the formation of oxygen vacancies is thermodynamically more favourable on the surface than in the bulk; it increases the electronic conductivity of reduced LaNiO3 in accordance with the enhanced OER activity that is observed.Peer ReviewedPostprint (author's final draft

Catalytic reduction of nitrogen to produce ammonia by bismuth-based catalysts: state of the art and future prospects

This review provides an up-to-date review on Bi-based nitrogen-fixation materials and future directions for the development of new Bi-based nitrogen-fixation materials under ambient conditions.</p

Orientation Growth and Magnetic Properties of Electrochemical Deposited Nickel Nanowire Arrays

Highly ordered ferromagnetic metal nanowire arrays with preferred growth direction show potential applications in electronic and spintronic devices. In this work, by employing a porous anodic aluminum oxide template-assisted electrodeposition method, we successfully prepared Ni nanowire arrays. Importantly, the growth direction of Ni nanowire arrays can be controlled by varying the current densities. The crystalline and growth orientation of Ni nanowire arrays show effects on magnetic properties. Single-crystallinity Ni nanowires with [110] orientation show the best magnetic properties, including coercivity and squareness, along the parallel direction of the nanowire axis. The current preparation strategy can be used to obtain other nanowire arrays (such as metal, alloy, and semiconductor) with controlled growth direction in confined space, and is therefore of broad interest for different applications

九州におけるソバ遺伝資源の諸特性の品種間差異および機能性の選抜法に関する研究

博士（農学）神戸大

A magnetically-separable H3PW12O40@Fe3O4/EN-MIL-101 catalyst for the one-pot solventless synthesis of 2H-indazolo[2,1-b] phthalazine-triones

A magnetic inorganic-organic catalyst, PTA@Fe3O4/EN-MIL-101 (EN = ethylenediamine, PTA = phosphotungstic acid) was fabricated and characterized by XRD, HRTEM, FESEM, UV–vis, TGA-DTA, FT-IR, XPS and porosimetry. PTA retained the parent Keggin structure upon dispersion throughout the amine-functionalized chromium terephthalate metal-organic framework, over which magnetic Fe3O4 nanoparticles were previously introduced. The resulting composite heterogeneous solid acid was an active catalyst for the one-pot synthesis of diverse 2H-indazolo[2,1-b] phthalazine-triones in good → excellent yields under mild, solventless condition, and offers facile separation and excellent recyclability

Advances in reforming and partial oxidation of hydrocarbons for hydrogen production and fuel cell applications

One of the most attractive routes for the production of hydrogen or syngas for use in fuel cell applications is the reforming and partial oxidation of hydrocarbons. The use of hydrocarbons in high temperature fuel cells is achieved through either external or internal reforming. Reforming and partial oxidation catalysis to convert hydrocarbons to hydrogen rich syngas plays an important role in fuel processing technology. The current research in the area of reforming and partial oxidation of methane, methanol and ethanol includes catalysts for reforming and oxidation, methods of catalyst synthesis, and the effective utilization of fuel for both external and internal reforming processes. In this paper the recent progress in these areas of research is reviewed along with the reforming of liquid hydrocarbons, from this an overview of the current best performing catalysts for the reforming and partial oxidizing of hydrocarbons for hydrogen production is summarized