Rapid consumption of fossil fuels (coal, oil, and natural gas) has caused a series of environmental hazards, thus exploring renewable and clean energies (e.g., H 2) is of great importance for the future development of sustainable society. [1] Owing to
The rise of micro-supercapacitors is satisfying the demand for power storage in portable devices and wireless gadgets. But the miniaturization of the energy-storage components is significantly limited by their energy density. Electrode materials with adequate electrochemical active surfaces are therefore required for improving performance. 2D materials with ultralarge specific surface areas offer a broad portfolio of the development of high-performance micro-supercapacitors in spite of their several critical drawbacks. An architecture engineering strategy is therefore developed to break these natural limits and maximize the significant advantages of these materials. Based on the approaches of phase transformation, intercalation, surface modification, material hybridization, and hierarchical structuration, 2D architectures with improved conductivity, enlarged specific surface, enhanced redox activity, as well as the unique synergetic effect exhibit great promise in the application of miniaturized supercapacitors with highly enhanced performance. Herein, the architecture engineering of emerging 2D materials beyond graphene toward optimizing the performance of micro-supercapacitors is discussed, in order to promote the application of 2D architectures in miniaturized energy-storage devices.
Photoelectrochemical reaction is emerging as a powerful approach for biomass conversion. However, it has been rarely explored for glucose conversion into value-added chemicals. Here we develop a photoelectrochemical approach for selective oxidation of glucose to high value-added glucaric acid by using single-atom Pt anchored on defective TiO2 nanorod arrays as photoanode. The defective structure induced by the oxygen vacancies can modulate the charge carrier dynamics and band structure, simultaneously. With optimized oxygen vacancies, the defective TiO2 photoanode shows greatly improved charge separation and significantly enhanced selectivity and yield of C6 products. By decorating single-atom Pt on the defective TiO2 photoanode, selective oxidation of glucose to glucaric acid can be achieved. In this work, defective TiO2 with single-atom Pt achieves a photocurrent density of 1.91 mA cm−2 for glucose oxidation at 0.6 V versus reversible hydrogen electrode, leading to an 84.3 % yield of glucaric acid under simulated sunlight irradiation.
The development of cost‐effective and highly efficient electrocatalysts to accelerate distinct electrochemical reactions is essential to help the industry to achieve a low‐carbon footprint. Single‐atom alloys (SAAs) with the characteristics of unique electronic structures, well‐defined active sites, and maximum atom utilization demonstrate promising potential to replace traditional noble metal catalysts. SAAs are expected to tailor the adsorption properties of reaction species, thus promoting electrocatalytic behaviors. Herein, representative synthetic strategies including wet chemistry, galvanic replacement, dealloying, and atomic layer deposition are introduced, followed by a summary of applications of SAAs in hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, carbon dioxide reduction reaction, and ethanol electro‐oxidation to provide an in‐depth understanding of the structure–activity relationship. Moreover, the challenges and perspectives in this emerging field of SAAs are discussed.
Highly efficient electrocatalysts play an integral part in developing renewable energy conversion and storage technologies. Despite considerable efforts devoted to synthesizing electrocatalysts with superior performance, the identification of active moieties and understanding of reaction mechanisms under practical conditions still remain elusive. Herein, the substantial progresses in unraveling the local electronic and atomic structure optimizations of nanocatalysts for gas‐involved electrocatalysis, disclosing real active sites, and clarifying their relationships with intrinsic activities by combining advanced characterization techniques with computational simulations are summarized. The continuous development of in situ and ex situ characterization tools, particularly at multi‐scale resolution, to monitor or even directly observe the active center structure is systematically discussed, which is divided into four main categories based on the type of active sites: atomically dispersed active sites, vacancies, heteroatom doping sites, and edge sites. Current challenges and perspectives in both fundamental area and industrial application are finally proposed for the future research direction of next‐generation electrode materials. The aim of this review is to provide mechanistic insights into the real catalytically active structure with the assistance of newly developed characterization techniques, guiding the rational design and structure engineering of advanced functional materials with outstanding activity, selectivity, and durability.
Owing to its unique atomic arrangement and electronic structure, metallic glass (MG) has been widely investigated in the field of energy storage and conversion. In the past few decades, multiple strategies have been developed to synthesize bulk and nanosized MG based materials. Here, combining the structure–activity relationship of MG with electrochemical reaction kinetics, the substantial progress of glass structures in electrocatalytic processes are highlighted, including the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, methanol oxidation reaction, carbon dioxide reduction reaction, and nitrogen fixation. Meanwhile, applications of MG materials in energy storage devices, like supercapacitors and lithium‐ion batteries, are also introduced in detail. Finally, challenges and possibilities for reasonable design of highly‐efficient MG‐based electrode materials are proposed. The integration of high‐throughput methods, artificial intelligence technology, as well as advanced characterization techniques is fundamental to screen materials with remarkable performance. This review aims to deepen the understanding of the relationship between electronic structure and electrochemical performance, providing guidance for rational design of functional MG materials with outstanding activity, selectivity, and durability.
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