Publications by authors named "Haiqun Chen"

The oxygen evolution reaction catalyst triggering lattice oxygen-mediated mechanism (LOM) can break the activity limitation imposed by the adsorbate evolution mechanism scaling relationship. However, triggering LOM is challenging due to the thermodynamic disadvantages associated with lattice oxygen redox reactions. Here, a Lewis acid-modified layered double hydroxides (LDH) heterojunction catalyst (LDH/CrO) is designed.

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Despite the advancement of the Pt-catalyzed hydrogen evolution reaction (HER) through oxophilic metal-hydroxide surface hybridization, its stability in acidic solutions remains unsatisfactory. This is primarily due to excessive aggregation of active hydrogen, which hinders subsequent hydrogen desorption, coupled with the poor operational stability of metal hydroxides. In this study, we have designed Pt nanoparticles-modified NiFeCoCuCr high-entropy layered double hydroxides (Pt/HE-LDH) that exhibit exceptional catalytic activity toward HER in acidic electrolytes.

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Article Synopsis
  • Graphitic carbon nitride (g-CN) is emerging as a strong photocatalyst for environmental and energy applications due to its stability and appropriate band structure, but suffers from issues like aggregation and low surface area that reduce its efficiency.
  • Significant research is focused on improving g-CN by designing tailored morphologies and optimizing electronic properties through various synthesis methods.
  • The review highlights recent advancements in g-CN synthesis techniques and discusses future challenges and directions for enhancing its photocatalytic performance.
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Macro-assembled silicon-based films can be taken into account as a possible anode material for the lithium ion batteries (LIBs) in portable electronics. However, most previously proposed preparation strategies are labor-intensive, intricate, and not appropriate for large-scale manufacturing. Herein, a multifunctional flexible silicon/carbon nanotube/reduced graphene oxide (Si/CNT/rGO) film was fabricated by one-step coating method based on the lyotropic nematic liquid crystals of graphene oxide (GO).

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Repulsing Cl to reduce its negative effects during seawater electrolysis is a promising strategy to guard against the corrosion of high-valence metal sites. Herein, we synthesized FeP/NiP by a facile Br-induced partial phase transition strategy. This FeP/NiP possessed intensified built-in electric field (BEF) due to large work function difference (Δ), demonstrating outstanding OER and HER activity in alkaline freshwater/seawater solution and exhibiting a low cell voltage for an anion exchange membrane water electrolyzer (AEMWE) system.

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Precisely designing asymmetric active centers and exploring their electronic regulation effects to prepare efficient bifunctional single-atom catalysts (SACs) is important for boosting the practical applications of zinc-air batteries (ZABs). Herein, an effective strategy has been developed by introducing an axial S atom to the FeN active center, simultaneously assisted by pyrolyzing the graphene oxide (GO) sheathed zeolitic-imidazolate framework-8 (ZIF8) composite and constructing a three-dimensional (3D) porous framework with abundant FeNS moieties. This structure can accelerate the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics owing to the modulated electronic redistribution and -band center with a reduced energy barrier.

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Cost-effective electrocatalysts is a key constituent to establish the balance of cost and catalytic efficiency for oxygen evolution reaction (OER) via water electrolysis in the area of energy conversion and storage. NiFe phosphide decorated with trace amount of iridium (Ir) species in-situ grown on carbon cloth was prepared by a facile wet chemistry approach followed by a phosphorization post-treatment at a relative low temperature. The optimal electrocatalyst, Ir-NiFeP/CC, exhibits excellent OER activity, with an low overpotential of 190 mV at 10 mA cm for alkaline OER, and a desirable long-term durability over 90 h.

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Aqueous zinc-ion batteries have become a promising energy storage battery due to high theoretical specific capacity, abundant zinc resources and low cost. However, zinc dendrite growth and hydrogen evolution reaction limit their application. This study aims to improve the cycling performance and stability of aqueous zinc-ion batteries by improving the gel electrolyte.

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It offers bright prospects to develop non-Pt group metal (non-PGM) electrocatalysts in the area of energy storage and conversion. Herein, we reported a simple spatial isolation strategy to synthesize Co-based electrocatalysts, using partially substituted Zn atoms in a ZnCo-ZIF precursor. The "fence" effect that originated from the partially substituted Zn atoms can yield a better isolation of Co atoms, achieving selective loading of Co species on nitrogen-doped porous carbon varying from nanoparticles to single atoms.

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The core principles of multicomponent interface and electronic structure engineering are essential in designing high-performance catalysts for the oxygen evolution reaction (OER). However, combining these aspects within a catalyst is a significant challenge. In this investigation, a novel approach involving the development of hybrid Ir-doped CoMO-Co(OH) (M = W and Mo) hollow nanoboxes was introduced, enabling remarkably efficient water oxidation electrocatalysis.

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Article Synopsis
  • * Researchers developed a three-dimensional self-supported heterostructure named FeCoMoS/CP using a hydrothermal method and vulcanization, enhancing catalytic activity due to its structural integrity and more accessible active sites.
  • * The FeCoMoS/CP demonstrated impressive electrocatalytic performance, requiring only 257 mV and 280 mV overpotentials for oxygen and hydrogen evolution reactions respectively, and achieving a high cell voltage of 1.48 V with excellent stability in an alkaline electrolyzer setup.
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Tailoring the dynamic reconstruction of transition metal compounds into highly active oxyhydroxides through surface electron state modification is crucial for advancing water oxidation, yet remains a formidable challenge. In this study, a unique polyaniline (PANI) electron bridge was integrated into the metal-organic frameworks (MOFs)/layer double hydroxides (LDHs) heterojunction to expedite electron transfer from MOFs to LDHs, facilitating electron accumulation at the metal sites within MOF and electron-deficient LDHs. This configuration promotes the surface dynamic reconstruction of LDHs into highly active oxyhydroxides while safeguarding the MOF from corrosion in harsh environments over extended periods.

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Metal-organic frameworks (MOFs) are normally moisture-sensitive and unstable in aqueous environments, which has considerably limited their practical applications because water/moisture is ubiquitous in many industrial processes. New materials with superior water stability are, therefore, in great demand and vital to their practical applications. Here, a novel oil/water interfacial assembly strategy is demonstrated for the synthesis of a new class of metal-organic monoacid framework (MOmAF) with exceptional water stability and chemical stability.

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Establishing homojunctions at the molecular level between different but physicochemically similar phases belonging to the same family of materials is an effective approach to promoting the photocatalytic activity of polymeric carbon nitride (CN) materials. Here, we prepared a CN material with a uniform distribution of homojunctions by combining two synthetic strategies: supramolecular assemblies as the precursor and molten salt as the medium. We designed porous CN rods with triazine-heptazine homojunctions (THCNs) using a melem supramolecular aggregate (Me) and melamine as the precursors and a KCl/LiBr salt mixture as the liquid reaction medium.

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Regulating the asymmetric active center of a single-atom catalyst to optimize the binding energy is critical but challenging to improve the overall efficiency of the electrocatalysts. Herein, an effective strategy is developed by introducing an axial hydroxyl (OH) group to the Fe─N center, simultaneously assisting with the further construction of asymmetric configurations by replacing one N atom with one S atom, forming FeNS─OH configuration. This novel structure can optimize the electronic structure and d-band center shift to reduce the reaction energy barrier, thereby promoting oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalytic activities.

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The electrocatalytic NO reduction reaction (NORR) to NH provides a promising pathway for ambient NH synthesis and environmental pollution treatment. Cu and its oxides are recognized as effective NORR electrocatalysts due to their favorable d-orbital energy levels and superior kinetics. In this work, mixed-valence Cu-based catalysts with tunable valence states were constructed an inorganic salt-induced MOF-derived strategy.

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The development of high-performing cathode materials for aqueous zinc-ion batteries (ZIBs) is highly important for the future large-scale energy storage. Owing to the distinctive framework structure, diversity of valences, and high electrochemical activity, spinel materials have been widely investigated and used for aqueous ZIBs. However, the stubborn issues of low electrical conductivity and sluggish kinetics plague their smooth applications in aqueous ZIBs, which stimulates the development of effective strategies to address these issues.

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Catalysts with an open hollow structure can enhance the mass transfer capability of the catalyst during the reaction process, thereby further improving the catalytic performance. In this work, uniform and monodisperse flying-squircher-shaped Al-MOFs were synthesized via a solvothermal method. Furthermore, a hollow structure AlO-supported metallic Ni catalyst (termed Ni-AlO-HFA) was synthesized via the Kirkendall effect for the hydrogenation-alkylation cascade reaction by employing as-synthesized Al-MOFs as a carrier for impregnation of Ni(NO)·6HO through further calcination and reduction.

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The nanocomposite gel system has been successfully applied as a water shutoff agent to enhance oil recovery (EOR) or for plugging to control lost circulation events. In this study, the silica/polyacrylamide nanocomposite was synthesized via in situ free radical polymerization of acrylamide (AM) monomers in the presence of silica nanoparticles. The composite was cross-linked with polyethylenimine to prepare a high-strength hydrogel.

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Through in-depth study of the properties and reaction mechanisms of catalysts, it is possible to better optimize catalytic systems and improve reaction efficiency and selectivity. This remains one of the challenges in the field of catalysis. Therefore, the research and design of catalysts play crucial roles in understanding and optimizing catalytic reaction mechanisms.

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The coordination of the electronic structure and charge transfer through heteroatomic doping and sulfur vacancies is one of the most vital strategies for enhancing the electrocatalytic performance of the oxygen and hydrogen evolution reactions (OER, HER) through water splitting. Se-doped CuCoS nanosheets (CuCoSSe) with abundant sulfur vacancies were synthesized a simple hydrothermal method to achieve remarkably efficient electrocatalytic water splitting. Importantly, incorporating Se in three-dimensional nanosheet structures effectively fine-tunes the electronic structure, ensuring ample accessibility of active sites for swift charge carrier transfer and improved reaction kinetics.

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Exploring efficient, easy-to-manufacture, and inexpensive bifunctional electrocatalysts with abundant accessible active sites is crucial for rechargeable zinc-air batteries (ZABs). Herein, we report the strategy consisting of the space confinement and pore-making engineering to fabricate single-atom catalyst enriched with Fe-N sites anchored on N-doped hierarchically porous carbon (Fe-NC-CN). The optimized Fe-NC-CN exhibits excellent oxygen reduction/evolution reaction (ORR/OER) activities with a half-wave potential (E) of 0.

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The development of innovative and efficient Fe-N-C catalysts is crucial for the widespread application of zinc-air batteries (ZABs), where the inherent oxygen reduction reaction (ORR) activity of Fe single-atom sites needs to be optimized to meet the practical application. Herein, a three-dimensional (3D) hollow hierarchical porous electrocatalyst (ZIF8@FePMPDA-920) rich in asymmetric Fe-N -OH moieties as the single atomic sites is reported. The Fe center is in a penta-coordinated geometry with four N atoms and one O atom to form Fe-N -OH configuration.

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Zinc-ion batteries are one of the promising energy storage devices, which have the advantages of environmental friendliness, high safety and low price and are expected to be used in large-scale battery application fields. However, four prominent water-induced adverse reactions, including zinc dendrite formation, zinc corrosion, passivation and the hydrogen evolution reaction in aqueous systems, seriously shorten the cycling life of zinc-ion batteries and greatly hinder their development. Based on this, polymer gel electrolytes have been developed to alleviate these issues due to their unique network structure, which can reduce water activity and suppress water-induced side reactions.

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Metallenes exhibit great potential for catalytic reaction, particularly for the hydrogen evolution reaction (HER) and biomass oxidation reaction, due to their favorable electronic configurations, ultrahigh specific surface areas, and highly accessible surface atoms. Therefore, metallenes can function as bifunctional electrocatalysts to boost the energy-saving biomass-oxidation-assisted HER, and have attracted great interest. Given the growing importance of green hydrogen as an alternative energy source in recent years, it is timely and imperative to summarize the recent progress and current status of metallene-based catalysts for the biomass-oxidation-assisted HER.

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