Publications by authors named "Qiu Jieshan"

Interfacial solar vapor generation (ISVG) accompanied by photocatalytic degradation holds immense potential to mitigate water scarcity and pollution. Distinct from the two detached functional components (photothermal agent and photocatalyst) in a conventional evaporator, in this study, an all-in-one photothermal/catalytic agent, nitrogen-containing honeycomb carbon nanosheets (NHC), was engineered for synergistic high-efficiency steam generation and photocatalysis functions. It was demonstrated that the superoxide radical generated on the surface of NHC conferred its catalytic activity to the photodegradation of organic pollutants under full solar spectrum irradiation.

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The past decades have witnessed the increasing accumulation of plastics, posing a daunting environmental crisis. Among various solutions, converting plastics into value-added products presents a significant endeavor. Here, an electrocatalytic upcycling route that efficiently converts waste poly(butylene terephthalate) plastics into high-value succinic acid with high Faradaic efficiency of 94.

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Membrane-assisted direct seawater splitting (DSS) technologies are actively studied as a promising route to produce green hydrogen (H), whereas the indispensable use of supporting electrolytes that help to extract water and provide electrochemically-accelerated reaction media results in a severe energy penalty, consuming up to 12.5 % of energy input when using a typical KOH electrolyte. We bypass this issue by designing a zero-gap electrolyzer configuration based on the integration of cation exchange membrane and bipolar membrane assemblies, which protects stable DSS operation against the precipitates and corrosion in the absence of additional supporting electrolytes.

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Article Synopsis
  • Carbon-based materials with a good balance of defects and microcrystals show potential as effective anode materials for sodium-ion batteries (SIBs), offering better capacity and conductivity.
  • The molecular chemistry technique involving cross-linking and defect repair helps manage the trade-off between active sites and conductivity limitations in these materials.
  • The resulting carbon material improves ion transfer and increases capacity significantly, from 162.5 to 336.5 mAh g, demonstrating a successful approach to enhancing SIB performance through microstructural regulation.
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Oriented zinc (Zn) electrodeposition is critical for the long-term performance of aqueous Zn metal batteries. However, the intricate interfacial reactions between the Zn anode and electrolytes hinder a comprehensive understanding of Zn metal deposition. Here, the reaction pathways of Zn deposition and report the preferential formation of Zn single-crystalline nuclei followed by dense Zn(002) deposition is elucidated, which is induced by a gradient solid-electrolyte interphase (SEI).

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Article Synopsis
  • Single-atom metals (SAMs), like Sn-SAMs, face challenges in catalytic performance due to low metal loading; this study introduces a method to create ultrahigh-loading Sn-SAMs on a carbon nanorings matrix.
  • The formation process involves converting oxygen-coordinated SnO to nitrogen-coordinated Sn-N while promoting diffusion throughout the carbon matrix using gaseous intermediates.
  • The resulting Sn-SAMs@CNR shows impressive performance in sodium-ion batteries, with high durability and a minimal capacity decay over extensive cycling, suggesting a promising strategy for enhancing energy storage materials.
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Although zeolitic imidazolate frameworks (ZIFs) possess the merits of orderly porosity, high permeability, and easy functionalization, the transformation of ZIFs into the real active species and the promotion of the catalytic efficiency and stability are still challenging. Herein, CoMo-based three-dimensional (3D) hollow nanocages composed of interconnected nanosheets are fabricated by in-situ etching metal-organic framework (ZIF-67) under the aid of MoO. X-ray photoelectron spectroscopy (XPS) and in-situ Raman confirm that Mo leaching can accelerate surface reconstruction and generate CoOOH active sites after continuous oxidation.

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2,5-Furandicarboxylic acid (FDCA), a critical polymer platform molecule that can potentially replace terephthalic acid, coupled hydrogen coproduction holds great prospects via electrolysis. However, the electrosynthesis of FDCA faces challenges in product separation from complex electrolytes and unclear electrochemical and nonelectrochemical reactions during the 5-hydroxymethylfurfural (HMF) oxidation. Herein, an electrochemical/chemical integrated system of alkaline HMF-HO co-electrolysis is proposed, achieving distillation-free synthesis of high-purity FDCA by acidic separation/purification and hydrogen coproduction.

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Carbonaceous materials hold great promise for K-ion batteries due to their low cost, adjustable interlayer spacing, and high electronic conductivity. Nevertheless, the narrow interlayer spacing significantly restricts their potassium storage ability. Herein, hierarchical N, S co-doped exfoliated holey graphene (NSEHG) with ultrahigh pyridinic/pyrrolic N (90.

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The development of nanomaterials for energy storage and conversion has always been important. Layered double hydroxide (LDH) is a promising material due to its high capacity, tunable composition and easy synthesis. In this work, the morphology of NiCo-LDH is tuned with surfactants including sodium dodecyl sulfate (SDS) and cetyltrimethylammonium bromide (CTAB), and investigated the correlation between morphology and electrochemical properties.

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Two-dimensional (2D) nonlayered metal compounds with porous structure show broad application prospects in electrochemistry-related fields due to their abundant active sites, open ions/electrons diffusion channels, and faradaic reactions. However, scalable and universal synthesis of 2D porous compounds still remains challenging. Here, inspired by blowing gum, a metal-organic gel (MOG) rapid redox transformation (MRRT) strategy is proposed for the mass production of a wide variety of 2D porous metal oxides.

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Seawater electrolysis for the production of fuels and chemicals involved in onshore and offshore plants powered by renewable energies offers a promising avenue and unique advantages for energy and environmental sustainability. Nevertheless, seawater electrolysis presents long-term challenges and issues, such as complex composition, potential side reactions, deposition of and poisoning by microorganisms and metal ions, as well as corrosion, thus hindering the rapid development of seawater electrolysis technology. This review focuses on the production of value-added fuels (hydrogen and beyond) and fine chemicals through seawater electrolysis, as a promising step towards sustainable energy development and carbon neutrality.

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Defect engineering and nitrogen doping being effective strategies for modulating the surface chemical state of the carbon matrix have been widely explored to promote the catalytic activity in the territory of electrochemical energy storage and conversion devices. However, the controllable synthesis of carbon material with high-density specific defects and high nitrogen doping is still full of challenges. Here, we first synthesize one-dimensional necklace-like nitrogen-doped carbon nanochains (N-CNCs) with abundant defects on carbon fiber paper (CFP) by chemical vapor deposition (CVD) method.

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Efficient production of value-added chemicals with high selectivity from CO electroreduction at industrial-level current density is highly demanded, yet remains a big challenge. In a recent issue of Angewandte Chemie, Han and colleagues have elegantly increased the Faradaic efficiency (FE) of multi-carbon (C) products to over 70 % at amperes level (1.4 A cm) by engineering the active sites for the key reactions involved in the CO electroreduction.

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Supermolecular hydrogel ionic skin (i-skin) linked with smartphones has attracted widespread attention in physiological activity detection due to its good stability in complex scenarios. However, the low ionic conductivity, inferior mechanical properties, poor contact adhesion, and insufficient freeze resistance of most used hydrogels limit their practical application in flexible electronics. Herein, a novel multifunctional poly(vinyl alcohol)-based conductive organohydrogel (PCEL) with a supermolecular structure was constructed by innovatively employing sodium carboxymethyl cellulose (CMC-Na) as reinforcement material, ethylene glycol as antifreeze, and lithium chloride as a water retaining agent.

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Prussian blue analogs (PBAs) are considered as one of the most potential electrode materials in capacitive deionization (CDI) due to their unique 3D framework structure. However, their practical applications suffer from low desalination capacity and poor cyclic stability. Here, an entropy engineering strategy is proposed that incorporates high-entropy (HE) concept into PBAs to address the unfavorable multistage phase transitions during CDI desalination.

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Nuclear power plays a pivotal role in the global energy supply. The adsorption-based extraction of uranium from seawater is crucial for the rapid advancement of nuclear power. The phosphorus nitride imide (PN) nanotubes were synthesized in this study using a solvothermal method, resulting in chemically stable cross-linked tubular hollow structures that draw inspiration from the intricate snowflake fractal pattern.

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The fine regulation of catalysts by the atomic-level removal of inactive atoms can promote the active site exposure for performance enhancement, whereas suffering from the difficulty in controllably removing atoms using current micro/nano-scale material fabrication technologies. Here, we developed a surface atom knockout method to promote the active site exposure in an alloy catalyst. Taking CuPd alloy as an example, it refers to assemble a battery using CuPd and Zn as cathode and anode, the charge process of which proceeds at about 1.

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The controlled conformational changes of planar graphene nanosheets are of great importance to the realization of their practical applications. Despite substantial effort in the area, the controlled folding of two-dimensional (2D) graphene sheets into one-dimensional (1D) structures still remains a significant challenge. Here, for the first time, we report an ice crystal guided folding strategy to fabricate 1D folded graphene nanobelts (FGBs), where the formation and growth of ice crystals in a confined space function to guide the folding of 2D graphene oxide (GO) nanosheets into 1D nanobelts ( folded graphene oxide belts, FGOBs), which were subsequently converted to FGBs after annealing.

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Electrooxidation of biomass into fine chemicals coupled with energy-saving hydrogen production for a zero-carbon economy holds great promise. Advanced anode catalysts determine the cell voltage and electrocatalytic efficiency greatly, further the rational design and optimization of their active site coordination remains a challenge. Herein, a phosphorus-oxygen terminals-rich species (NiP-O-300) via an anion-assisted pyrolysis strategy is reported to induce strong electronic coupling and high valence state of active nickel sites over nickel phosphide.

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As one of the key components of supercapacitors, electrolyte is intensively investigated to promote the fast development of the energy supply system under extremely cold conditions. However, high freezing point and sluggish ion transport kinetics for routine electrolytes hinder the application of supercapacitors at low temperatures. Resultantly, the liquid electrolyte should be oriented to reduce the freezing point, accompanied by other superior characteristics, such as large ionic conductivity, low viscosity and outstanding chemical stability.

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Carbon materials with hierarchical porous structures hold great potential for redox electrolyte-enhanced supercapacitors. However, restricted by the intrinsic inert and nonpolar characteristics of carbon, the energy barrier of anchoring redox electrolytes on the pore walls is relatively high. As such, the redox process at the interface less occurs, and the rate of mass transfer is impaired, further leading to a poor electrochemical performance.

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Green ammonia (NH), made by using renewable electricity to split nearly limitless nitrogen (N) molecules, is a vital platform molecule and an ideal fuel to drive the sustainable development of human society without carbon dioxide emission. The NH electrosynthesis field currently faces the dilemma of low yield rate and efficiency; however, decoupling the overlapping issues of this area and providing guidelines for its development directions are not trivial because it involves complex reaction process and multidisciplinary entries (for example, electrochemistry, catalysis, interfaces, processes, etc.).

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Conventional H-O fuel cells suffer from the low output voltage, insufficient durability, and high-cost catalysts (e.g., noble metals).

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