: The unpolarized absorption and circular dichroism spectra of the fundamental vibrational transitions of the chiral molecule, 4-methyl-2-oxetanone, are calculated ab initio. Harmonic force fields are obtained using Density Functional Theory (DFT), MP2, and SCF methodologies and a 5S4P2D/3S2P (TZ2P) basis set. DFT calculations use the Local Spin Density Approximation (LSDA), BLYP, and Becke3LYP (B3LYP) density functionals. Mid-IR spectra predicted using LSDA, BLYP, and B3LYP force fields are of significantly different quality, the B3LYP force field yielding spectra in clearly superior, and overall excellent, agreement with experiment. The MP2 force field yields spectra in slightly worse agreement with experiment than the B3LYP force field. The SCF force field yields spectra in poor agreement with experiment.The basis set dependence of B3LYP force fields is also explored: the 6-31G* and TZ2P basis sets give very similar results while the 3-21G basis set yields spectra in substantially worse agreements with experiment. jg

Ab initio calculation of vibrational absorption and circular dichroism spectra using density functional force fields

This review offers a focused discussion on the recent progress of biomass-derived nitrogen-doped porous carbon (NPC) and its applications. Various synthesis methods for biomass-derived NPCs are introduced and critically reviewed. N-doping is a promising approach for further improving the physicochemical/electrochemical properties of carbon materials. Besides, NPC synthesis from inexpensive biomass for energy storage applications is a green and sustainable strategy. NPCs can be synthesized directly from algae, chitosan, and glucosamine without using any additional N precursor. The effect of synthesis methods on the physicochemical properties of NPCs offers a direction for optimizing the properties of NPCs for diverse applications. The utilization of NPCs in various applications, including catalysis and electrochemical energy storage (e.g., fuel cells, batteries, and supercapacitors), is reviewed. Besides, a discussion on the use of NPCs in oxidation and hydrogenation reactions, CO2 capture and reduction is provided. The factors controlling the electrocatalytic performance of NPC are evaluated, such as the effect of N-content and the type of N species in NPCs. Finally, to improve the rational design of biomass-derived NPCs for catalysis and energy storage applications, an outlook and conclusion are provided.

Recent progress in the development of biomass-derived nitrogen-doped porous carbon

Transformation of biomass to chemicals and fuels is a long-term goal in both science and industry. However, high cost is one of the major obstacles to the industrialization of this sustainable technology. Thus, developing catalysts with high activity and low-cost is of great importance for biomass conversion. The last two decades have witnessed the increasing achievement of the use of earth-abundant 3d-transition-metals in catalysis due to their low-cost, high efficiency and excellent stability. Here, we aim to review the fast development and recent advances of 3d-metal-based catalysts including Cu, Fe, Co, Ni and Mn in lignocellulosic biomass conversion. Moreover, present research trends and invigorating perspectives on future development are given.

Earth-abundant 3d-transition-metal catalysts for lignocellulosic biomass conversion

Zeolitic imidazolate frameworks derived Fe1-N-C catalysts with isolated single iron atoms have been synthesized and applied for selective ammoxidation reactions. For the preparation of the different Fe-based materials, benzylamine as an additive proved to be essential to tune the morphology and size of ZIFs resulting in uniform and smaller particles, which allow stable atomically dispersed Fe-N4 active sites. The optimal catalyst Fe1-N-C achieves an efficient synthesis of various aryl, heterocyclic, allylic, and aliphatic nitriles from alcohols in water under very mild conditions. With its chemoselectivity, recyclability, high efficiency under mild conditions this new system complements the toolbox of catalysts for nitrile synthesis, which are important intermediates with many applications in life sciences and industry. 

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Efficient iron single-atom catalysts for selective ammoxidation of alcohols to nitriles

The Lewis/Bronsted catalytic properties of the Metal-Organic Framework (MOF) nodes can be tuned by simply controlling the solvent employed in the synthetic procedure. In this work, we demonstrate that Hf-MOF-808 can be prepared from a material with a higher amount of Bronsted acid sites, via modulated hydrothermal synthesis, to a material with a higher proportion of unsaturated Hf Lewis acid sites, via modulated solvothermal synthesis. The Lewis/Bronsted acid properties of the resultant metallic clusters have been studied by different characterization techniques, including XAS, FTIR and NMR spectroscopies, combined with a DFT study. The different nature of the Hf-MOF-808 materials allows their application as selective catalysts in different target reactions requiring Lewis, Bronsted or Lewis-Bronsted acid pairs.

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Tailoring Lewis/Brønsted acid properties of MOF nodes via hydrothermal and solvothermal synthesis: simple approach with exceptional catalytic implications.

Porous cobalt@N-doped carbon derived from chitosan for oxidative esterification of 5-Hydroxymethylfurfural: The roles of zinc in the synthetic and catalytic process

Baojing Zhou

Papers

Porous cobalt@N-doped carbon derived from chitosan for oxidative esterification of 5-Hydroxymethylfurfural: The roles of zinc in the synthetic and catalytic process

Hf-MOF catalyzed Meerwein−Ponndorf−Verley (MPV) reduction reaction: Insight into reaction mechanism

A DFT study on the mechanism of rhodium-catalyzed regioselective hydrothiolation of the allyl amine