Macromolecules最新文献

Catalytic CO_x (CO and CO₂) hydrogenation to valued chemicals is one of the promising approaches to address challenges in energy, environment, and climate change. H₂O is an inevitable side product in these reactions, where its existence and effect are often ignored. In fact, H₂O significantly influences the catalytic active centers, reaction mechanism, and catalytic performance, preventing us from a definitive and deep understanding on the structure-performance relationship of the authentic catalysts. It is necessary, although challenging, to clarify its effect and provide practical strategies to tune the concentration and distribution of H₂O to optimize its influence. In this review, we focus on how H₂O in CO_x hydrogenation induces the structural evolution of catalysts and assists in the catalytic processes, as well as efforts to understand the underlying mechanism. We summarize and discuss some representative tuning strategies for realizing the rapid removal or local enrichment of H₂O around the catalysts, along with brief techno-economic analysis and life cycle assessment. These fundamental understandings and strategies are further extended to the reactions of CO and CO₂ reduction under an external field (light, electricity, and plasma). We also present suggestions and prospects for deciphering and controlling the effect of H₂O in practical applications.

Hydrogen–deuterium exchange (HDX) has become a pivotal method for investigating the structural and dynamic properties of proteins. The versatility and sensitivity of mass spectrometry (MS) made the technique the ideal companion for HDX, and today HDX-MS is addressing a growing number of applications in both academic research and industrial settings. The prolific generation of experimental data has spurred the concurrent development of numerous computational tools, designed to automate parts of the workflow while employing different strategies to achieve common objectives. Various computational methods are available to perform automated peptide searches and identification; different statistical tests have been implemented to quantify differences in the exchange pattern between two or more experimental conditions; alternative strategies have been developed to deconvolve and analyze peptides showing multimodal behavior; and different algorithms have been proposed to computationally increase the resolution of HDX-MS data, with the ultimate aim to provide information at the level of the single residue. This review delves into a comprehensive examination of the merits and drawbacks associated with the diverse strategies implemented by software tools for the analysis of HDX-MS data.

In this contribution, we review the electrochemical upgrading of saccharides (e.g., glucose) and sugar alcohols (e.g., glycerol) on metal and metal-oxide electrodes by drawing conclusions on common trends and differences between these two important classes of biobased compounds. For this purpose, we critically review the literature on the electrocatalytic oxidation of saccharides and sugar alcohols, seeking trends in the effect of reaction conditions and electrocatalyst design on the selectivity for the oxidation of specific functional groups toward value-added compounds. Importantly, we highlight and discuss the competition between electrochemical and non-electrochemical pathways. This is a crucial and yet often neglected aspect that should be taken into account and optimized for achieving the efficient electrocatalytic conversion of monosaccharides and related sugar alcohols into valuable products, which is a target of growing interest in the context of the electrification of the chemical industry combined with the utilization of renewable feedstock.