Tuning the Adsorption Energy of Methanol Molecules Along Ni‐N‐Doped Carbon Phase Boundaries by the Mott–Schottky Effect for Gas‐Phase Methanol Dehydrogenation

Abstract

Engineering the adsorption of molecules on active sites is an integral and challenging part for the design of highly efficient transition‐metal‐based catalysts for methanol dehydrogenation. A Mott–Schottky catalyst composed of Ni nanoparticles and tailorable nitrogen‐doped carbon‐foam (Ni/NCF) and thus tunable adsorption energy is presented for highly efficient and selective dehydrogenation of gas‐phase methanol to hydrogen and CO even under relatively high weight hourly space velocities (WHSV). Both theoretical and experimental results reveal the key role of the rectifying contact at the Ni/NCF boundaries in tailoring the electron density of Ni species and enhancing the absorption energies of methanol molecules, which leads to a remarkably high turnover frequency (TOF) value (356 mol methanol mol−1 Ni h−1 at 350 °C), outpacing previously reported bench‐marked transition‐metal catalysts 10‐fold.

Electrochemical Reduction of N2 into NH3 by Donor–Acceptor Couples of Ni and Au Nanoparticles with a 67.8% Faradaic Efficiency

“…SEM and TEM observation (Figures S2−S3) further indicated similar foam-like structures for the carbon supports decorated with metal nanoparticles (mean size: ∼17 nm) for the different Au x /Ni samples. The XRD patterns directly identify the presence of metallic Ni and Au nanoparticles (Figure 1c) 26 We initially evaluated the catalytic performance of the Au− Ni couple-based NRR electrocatalysts in an H-type cell (Figure S7). An obvious shift in the cyclic voltammetry (CV) curves of the Au/Ni samples, taking Au 6 /Ni sample to a lower potential, indicates a possible NRR in the electrolyte after saturation with N 2 gas to replace the Ar gas (Figure 2a).…”

Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol

“…Notably, the Cu AES shifted to the higher kinetic energy with the potential reduced, indicating fewer electrons on average Cu were transferred to the nitrogen-doped carbon support of the −1.2 V vs. RHE. The catalysis electron configuration would obviously affect the adsorption of the non-polar molecule, which played an important role during the reduction process 39,40 . Probably, the ethanol productivity declined at −1.2 V vs. RHE, because the larger cluster could lead to the Cu 0 electron configuration increasing 32,41 .…”

Reaction Packaging CoSe2 Nanoparticles in N-Doped Carbon Polyhedra with Bifunctionality for Overall Water Splitting

“…Developing clean and renewable alternatives to fossil fuels is a matter of great urgency. − Among various of alternatives, hydrogen is regarded as most promising clean energy carriers because of its high energy density and environmentally friendly features. ,, Water electrolysis is the most efficient and large-scale strategy for the simultaneous production of hydrogen and oxygen. , The water electrolysis is composed of two basic reactions, namely, the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) . The sluggish kinetics of the two reactions greatly hinder energy conversion efficiency for overall water splitting. ,− Therefore, the development of efficient and durable bifunctional HER/OER catalysts is the key to achieve high energy efficiency for an electrolyzer.…”