Development of large-scale alkaline seawater electrolysis requires robust and corrosion-resistant anodes. Here we propose engineering NiFe layered double hydroxide (LDH)-based anodes by incorporating a series of anions into the LDH interlayers. The most optimal NiFe LDH anode with intercalated phosphates demonstrates stable operation at a high current density of 1.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2024
Currently, direct electrolysis of seawater for green hydrogen production is primarily focused on neutral and alkaline systems. However, the precipitation of calcium and magnesium ions restricts the advancement of this technology. An acidic system can effectively address this issue.
View Article and Find Full Text PDFElectrolysis of natural seawater driven by renewable energy is practically attractive for green hydrogen production. However, because precipitation initiated by an increase in local pH near to the cathode deactivates catalysts or blocks electrolyzer channels, limited catalysts are capable of operating with untreated, natural seawater (., pH 8.
View Article and Find Full Text PDFThis perspective summarizes the understanding about the local reaction environment in the electrocatalysis and underscores the influence of local environment due to its special location.
View Article and Find Full Text PDFCatalytic upcycling of plastic wastes offers a sustainable circular economy. Selective conversion of the most widely used polyester, polyethylene terephthalate (PET), under ambient conditions is practically attractive because of low energy consumption and carbon footprint. Here, we report selective, aerobic conversion of PET in a flow reactor using TiO photocatalyst modified with atomic Pd and metallic PdCu (PdCu-TiO) under ambient conditions.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Conventional water electrolysis relies on expensive membrane-electrode assemblies and sluggish oxygen evolution reaction (OER) at the anode, which makes the cost of green hydrogen (H) generation much higher than that of grey H. Here, we develop an innovative and efficient membrane-free water electrolysis system to overcome these two obstacles simultaneously. This system utilizes the thermodynamically more favorable urea oxidation reaction (UOR) to generate clean N over a new class of Cu-based catalyst (CuO) for replacing OER, fundamentally eliminating the explosion risk of H and O mixing while removing the need for membranes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Zinc-iodine (Zn-I) batteries are gaining popularity due to cost-effectiveness and ease of manufacturing. However, challenges like polyiodide shuttle effect and Zn dendrite growth hinder their practical application. Here, we report a cation exchange membrane to simultaneously prevent the polyiodide shuttle effect and regulate Zn deposition.
View Article and Find Full Text PDFCarbon-carbon (C-C) coupling is essential in the electrocatalytic reduction of CO for the production of green chemicals. However, due to the complexity of the reaction network, there remains controversy regarding the underlying reaction mechanisms and the optimal direction for catalyst material design. Here, we present a global perspective to establish a comprehensive data set encompassing all C-C coupling precursors and catalytic active site compositions to explore the reaction mechanisms and screen catalysts big data set analysis.
View Article and Find Full Text PDFThe development of all-solid-state lithium-sulfur batteries (ASSLSBs) toward large-scale electrochemical energy storage is driven by the higher specific energies and lower cost in comparison with the state-of-the-art Li-ion batteries. Yet, insufficient mechanistic understanding and quantitative parameters of the key components in sulfur-based cathode hinders the advancement of the ASSLSB technologies. This review offers a comprehensive analysis of electrode parameters, including specific capacity, voltage, S mass loading and S content toward establishing the specific energy (Wh kg) and energy density (Wh L) of the ASSLSBs.
View Article and Find Full Text PDFAqueous zinc-iodine (Zn-I) batteries hold potential for large-scale energy storage but struggle with shuttle effects of I cathodes and poor reversibility of Zn anodes. Here, an interfacial gelation strategy is proposed to suppress the shuttle effects and improve the Zn reversibility simultaneously by introducing silk protein (SP) additive. The SP can migrate bidirectionally toward cathode and anode interfaces driven by the periodically switched electric field direction during charging/discharging.
View Article and Find Full Text PDFAqueous zinc batteries are practically promising for large-scale energy storage because of cost-effectiveness and safety. However, application is limited because of an absence of economical electrolytes to stabilize both the cathode and anode. Here, we report a facile method for advanced zinc-iodine batteries via addition of a trace imidazolium-based additive to a cost-effective zinc sulfate electrolyte, which bonds with polyiodides to boost anti-self-discharge performance and cycling stability.
View Article and Find Full Text PDFThe exploration of post-Lithium (Li) metals, such as Sodium (Na), Potassium (K), Magnesium (Mg), Calcium (Ca), Aluminum (Al), and Zinc (Zn), for electrochemical energy storage has been driven by the limited availability of Li and the higher theoretical specific energies compared to the state-of-the-art Li-ion batteries. Post-Li metal||S batteries have emerged as a promising system for practical applications. Yet, the insufficient understanding of quantitative cell parameters and the mechanisms of sulfur electrocatalytic conversion hinder the advancement of these battery technologies.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2024
Electrocatalytic acetylene hydrogenation to ethylene (E-AHE) is a promising alternative for thermal-catalytic process, yet it suffers from low current densities and efficiency. Here, we achieved a 71.2 % Faradaic efficiency (FE) of E-AHE at a large partial current density of 1.
View Article and Find Full Text PDFAqueous zinc (Zn) batteries have attracted global attention for energy storage. Despite significant progress in advancing Zn anode materials, there has been little progress in cathodes. The predominant cathodes working with Zn/H intercalation, however, exhibit drawbacks, including a high Zn diffusion energy barrier, pH fluctuation(s) and limited reproducibility.
View Article and Find Full Text PDFAqueous sodium-ion batteries are practically promising for large-scale energy storage, however energy density and lifespan are limited by water decomposition. Current methods to boost water stability include, expensive fluorine-containing salts to create a solid electrolyte interface and addition of potentially-flammable co-solvents to the electrolyte to reduce water activity. However, these methods significantly increase costs and safety risks.
View Article and Find Full Text PDFBeyond conventional electrocatalyst engineering, recent studies have unveiled the effectiveness of manipulating the local reaction environment in enhancing the performance of electrocatalytic reactions. The general principles and strategies of local environmental engineering for different electrocatalytic processes have been extensively investigated. This review provides a critical appraisal of the recent advancements in local reaction environment engineering, aiming to comprehensively assess this emerging field.
View Article and Find Full Text PDFUrea is one of the most essential reactive nitrogen species in the nitrogen cycle and plays an indispensable role in the water-energy-food nexus. However, untreated urea or urine wastewater causes severe environmental pollution and threatens human health. Electrocatalytic and photo(electro)catalytic urea oxidation technologies under mild conditions have become promising methods for energy recovery and environmental remediation.
View Article and Find Full Text PDFCurrent chemical recycling of bulk synthetic plastic, polyethylene (PE), operates at high temperature/pressure and yields a complex mixture of products. PE conversion under mild conditions and with good selectivity toward value-added chemicals remains a practical challenge. Here, we demonstrate an atomic engineering strategy to modify a TiO photocatalyst with reversible Pd species for the selective conversion of PE to ethylene (CH) and propionic acid via dicarboxylic acid intermediates under moderate conditions.
View Article and Find Full Text PDFSci Bull (Beijing)
December 2023