Renewable energy and advanced water treatment technologies hold profound significance for driving sustainable development in modern society. Given the environmental friendliness and high efficiency of electrocatalysis processes, great expectations are placed on their applications in energy and water-related fields. However, the electrocatalysis is limited by the selectivity, activity, and durability of the electrocatalytic reactions.
View Article and Find Full Text PDFHigh-entropy alloys (HEAs) present both significant potential and challenges for developing efficient electrocatalysts due to their diverse combinations and compositions. Here, we propose a procedural approach that combines high-throughput experimentation with data-driven strategies to accelerate the discovery of efficient HEA electrocatalysts for the hydrogen evolution reaction (HER). This enables the rapid preparation of HEA arrays with various element combinations and composition ratios within a model system.
View Article and Find Full Text PDFThe electrochemical nitrate reduction reaction (NORR) holds promise for converting nitrogenous pollutants to valuable ammonia products. However, conventional electrocatalysis faces challenges in effectively driving the complex eight-electron and nine-proton transfer process of the NORR while also competing with the hydrogen evolution reaction. In this study, we present the thermally enhanced electrocatalysis of nitrate-to-ammonia conversion over nickel-modified copper oxide single-atom alloy oxide nanowires.
View Article and Find Full Text PDFSingle-atom catalysts (SACs), specifically iron single atoms dispersed on nitrogen-doped carbon (Fe-NC), have shown promising potential in the electrocatalytic reduction of nitrate to ammonia (NitRR), but there is a lack of understanding of their intrinsic activity. The conventional measurements often overlook the intrinsic performance of SACs, leading to significant underestimation. This study presents an in situ electrochemical probing protocol, using two poisoning molecules (SCN and NO), to characterize the reactivity of Fe sites in Fe-NC SACs for NitRR.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2024
The performance of aqueous Zn ion batteries (AZIBs) is hindered by the uncontrollable growth of Zn dendrites and side reactions at the Zn anode/electrolyte interface. Here, we introduce low-cost glucosamine hydrochloride (GLA) into the ZnSO electrolyte system to modulate the Zn anode/electrolyte interface and the solvation structure of Zn, which leads to improved reversibility of Zn plating/striping. Through experimental and theoretical analyses, we demonstrate that GLA molecules could adsorp on the Zn metal surface to form a new interface with reduced active water, effectively suppressing water-induced side reactions.
View Article and Find Full Text PDFThe selective two-electron electrochemical oxygen reduction reaction (ORR) for hydrogen peroxide (HO) production is a promising and green alternative method to the current energy-intensive anthraquinone process used in industry. In this study, we develop a single-atom catalyst (CNT-D-O-Fe) by anchoring defect-stabilized and oxygen-coordinated iron atomic sites (Fe-O) onto porous carbon nanotubes using a local etching strategy. Compared to O-doped CNTs with vacancy defects (CNT-D-O) and oxygen-coordinated Fe single-atom site modifying CNTs without a porous structure (CNT-O-Fe), CNT-D-O-Fe exhibits the highest HO selectivity of 94.
View Article and Find Full Text PDFDespite modern chemistry's success in providing affordable fertilizers for feeding the population and supporting the ammonia industry, ineffective nitrogen management has led to pollution of water resources and air, contributing to climate change. Here, we report a multifunctional copper single-atom electrocatalyst-based aerogel (Cu SAA) that integrates the multiscale structure of coordinated single-atomic sites and 3D channel frameworks. The Cu SAA demonstrates an impressive faradaic efficiency of 87% for NH synthesis, as well as remarkable sensing performance with detection limits of 0.
View Article and Find Full Text PDFAnthropogenic nitrate pollution has an adverse impact on the environment and human health. As part of a sustainable nitrate management strategy, electrochemical denitrification is studied as an innovative strategy for nutrients recycling and recovering. It is, however, challenging to selectively electro-reduce nitrate with low-concentration for ammonia.
View Article and Find Full Text PDFThe real-time measurement of the individual or local electrocatalytic reactivity of catalyst particles instead of ensemble behavior is considerably challenging but very critical to uncover fundamental insights into catalytic mechanisms. Recent remarkable efforts have been made to the development of high-spatiotemporal-resolution electrochemical techniques, which allow the imaging of the topography and reactivity of fast electron-transfer processes at the nanoscale. This Perspective summarizes emerging powerful electrochemical measurement techniques for studying various electrocatalytic reactions on different types of catalysts.
View Article and Find Full Text PDFElectroreduction of nitrate to ammonia offers a promising pathway for nutrient recycling and recovery from wastewater with energy and environmental sustainability. There have been considerable efforts on the regulation of reaction pathways to facilitate nitrate-to-ammonia conversion over the competing hydrogen evolution reaction but only with limited success. Here, we report a Cu single-atom gel (Cu SAG) electrocatalyst that produces NH from both nitrate and nitrite under neutral conditions.
View Article and Find Full Text PDFAs an emerging class of materials with distinctive physicochemical properties, metallenes are deemed as efficient catalysts for energy-related electrocatalytic reactions. Engineering the lattice strain, electronic structure, crystallinity, and even surface porosity of metallene provides a great opportunity to further enhance its catalytic performance. Herein, we rationally developed a reconstruction strategy of Pd metallenes at atomic scale to generate a series of nonmetallic atom-intercalated Pd metallenes (M-Pdene, M = H, N, C) with lattice expansion and S-doped Pd metallene (S-Pdene) with an amorphous structure.
View Article and Find Full Text PDFChem Commun (Camb)
May 2022
We report a wire-shaped bifunctional oxygen photoelectrode by integrating Li-doped TiO nanotubes and Pt nanoclusters. Conductive nanoshells have been identified at the lithiated interface of Pt/TiO, which facilitates the performance of oxygen catalysis. Thus, the assembled Zn-air micro-battery with solar-assisted charging greatly improves the voltage efficiency compared with the conventional state-of-the-art catalyst as the air electrode.
View Article and Find Full Text PDFGenomics Proteomics Bioinformatics
August 2022
After decades of development, protein and peptide drugs have now grown into a major drug class in the marketplace. Target identification and validation are crucial for the discovery of protein and peptide drugs, and bioinformatics prediction of targets based on the characteristics of known target proteins will help improve the efficiency and success rate of target selection. However, owing to the developmental history in the pharmaceutical industry, previous systematic exploration of the target spaces has mainly focused on traditional small-molecule drugs, while studies related to protein and peptide drugs are lacking.
View Article and Find Full Text PDFSingle-atom catalysts (SACs) have aroused tremendous interest over the past decade, particularly in the community of energy and environment-related electrocatalysis. A rapidly growing number of recent publications have recognized it as a promising candidate with maximum atomic utilization, distinct activity, and selectivity in comparison to bulk catalysts and nanocatalysts. However, the complexity of localized coordination environments and the dispersion of isolated sites lead to significant difficulties when it comes to gaining insight into the intrinsic behavior of electrocatalytic reactions.
View Article and Find Full Text PDFAmmonia (NH) is an essential ingredient in agriculture and a promising source of clean energy as a hydrogen carrier. The current major method for ammonia production, however, is the Haber-Bosch process that leads to massive energy consumption and severe environmental issues. Compared with nitrogen (N) reduction, electrochemical nitrate reduction reaction (NORR), with a higher NH yield rate and Faradaic efficiency, holds promise for efficient NH production under ambient conditions.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2021
Aqueous Ni/Fe alkaline batteries with features of low cost and high safety show great potential for application in portable and wearable electronics. However, the poor kinetics of the Fe-based anode greatly limits the large-scale applications of Ni/Fe batteries. Herein, we report an interconnected 3D conductive network with carbon-coated nanostructured iron/iron oxide (3D-Fe/FeO@C) as an efficient anode for a flexible Ni/Fe battery.
View Article and Find Full Text PDFObjective: B7-H3 is a member of the B7 family of immune checkpoint molecule. Although B7-H3 has been shown to regulate T cell-mediated peripheral immune response, whether it also correlated with NK cell exhaustion in ovarian cancer remains unclear. The purpose of this study was to explore the mechanism of B7-H3 regulating NK-cell proliferation and function.
View Article and Find Full Text PDFBacteria alter their local chemical environment through both consumption and the production of a variety of molecules, ultimately shaping the local ecology. Molecular oxygen (O) is a key metabolite that affects the physiology and behavior of virtually all bacteria, and its consumption often results in O gradients within sessile bacterial communities (biofilms). O plays a critical role in several bacterial phenotypes, including antibiotic tolerance; however, our understanding of O levels within and surrounding biofilms has been hampered by the difficulties in measuring O levels in real-time for extended durations and at the micron scale.
View Article and Find Full Text PDFEndometriosis (EMs) is defined as the presence of tissue which somewhat resembles endometrial glands and stroma outside the uterus, and elicits fibrosis. Fibrosis is the main factor resulting in pain and infertility, while the aetiology of endometrial fibrosis is unknown. There is strong evidence from numerous experiments showing that connective tissue growth factor (CCN2) plays a central role in fibrogenesis.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2020
A surface-strained and geometry-optimized TiO nanoreactor enhances the performance of electrocatalytic nitrogen fixation. The nanotubular confinement allows spatial regulation of the mass transport of nitrogen during the NRR process and offers an enlarged surface area, thus boosting the ammonia production with high selectivity. Both experimental and theoretical evidence support strained Ti sites, demonstrating a more favorable pathway for the N activation and selective NH production with a faster kinetic rate than the pristine TiO .
View Article and Find Full Text PDFSurface interrogation scanning electrochemical microscopy (SI-SECM) of two electrodeposited manganese-based electrocatalysts, amorphous MnO and perovskite CaMnO , was used to investigate the manganese oxidation state relating to the oxygen evolution reaction (OER) under neutral conditions. The results indicate the amounts of Mn and Mn species in MnO and CaMnO depend on potential. A Mn species was identified in both structures during the OER.
View Article and Find Full Text PDFWe report an electrodeposition protocol for preparing isolated cobalt oxide single molecules (CoO) and clusters (Co O) on a carbon fiber nanoelectrode. The as-prepared deposits are able to produce well-defined steady-state voltammograms for the oxygen evolution reaction (OER) in alkaline media, where the equivalent radius () is estimated by the limiting current of hydroxide oxidation in accordance with the electrocatalytic amplification model. The size of isolated clusters obtained from the femtomolar Co solution through an atom-by-atom technique can reach as small as 0.
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