Publications by authors named "Shi Zhang Qiao"

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.

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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.

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Electrolysis 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.

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This perspective summarizes the understanding about the local reaction environment in the electrocatalysis and underscores the influence of local environment due to its special location.

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Catalytic 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.

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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.

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Article Synopsis
  • The study focuses on improving the stability of aqueous Zn-ion batteries (AZIBs) by using electrolyte additives, moving away from traditional trial-and-error methods.
  • A data-driven approach is proposed, utilizing theoretically calculated surface free energy to create a database for machine learning (ML) training while relying on experimental data for better accuracy.
  • Key findings reveal that the number of heavy atoms and liquid surface tension in electrolyte additives play crucial roles; experimental results validate the effectiveness of specific additives like 1,2,3-butanetriol and acetone.
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  • Aqueous zinc-iodine batteries (ZIBs) are gaining popularity due to their efficient energy conversion and fast reaction rates, although the common two-electron types struggle with low energy density.
  • Recent advancements in four-electron ZIBs have improved energy density but face challenges with redox reversibility and issues like polyiodide shuttling.
  • The review discusses the mechanisms, limitations of ZIBs, emphasizes the importance of zinc utilization rates, and suggests solutions for recycling iodine electrodes to support sustainable energy storage.
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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.

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Carbon-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.

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The 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.

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Aqueous 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.

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Aqueous 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.

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The 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.

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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.

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Aqueous 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.

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Article Synopsis
  • * By using synchrotron X-ray adsorption and molecular orbital computations, the research highlights how the atomic structure of transition metal catalysts influences polysulfide levels and, ultimately, SRR kinetics.
  • * A newly designed nanocomposite electrocatalyst made of carbon and CoZn clusters is tested, achieving impressive performance in a sulfur-based battery setup, with 1,000 cycles at high current rates and significant energy retention.
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  • Over 8 billion tons of plastics have been produced since 1950, with around 80% ending up in landfills or natural environments, causing significant contamination.
  • Photocatalysis is highlighted as a promising method for recycling plastic waste, as it operates at mild conditions, using solar light to convert plastics into valuable chemicals and fuels.
  • The text reviews recent advancements in photocatalytic plastic upcycling, discussing different types of photocatalysts and their advantages/disadvantages, along with future challenges and opportunities in this field.
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Aqueous 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.

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Beyond 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.

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Urea 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.

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  • Researchers address the challenges of operating rechargeable batteries at ultralow temperatures, highlighting poor kinetics of the electrodes.
  • They introduce a novel organic electrode made from disodium rhodizonate and graphene oxide, achieving impressive performance with a capacity of 130 mAh g at -50 °C.
  • The full-cell design, using Prussian blue analogues, shows remarkable cycling stability over 7000 cycles at -40 °C, maintaining effective power supply even in extreme cold.
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Current 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.

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