Publications by authors named "Zhao-qing Liu"

Porous organic polymers have shown great potential in photocatalytic CO2 reduction due to their unique tunable structure favoring gas adsorption and metal sites integration. However, efficient photocatalysis in porous polymers is greatly limited by the low surface reactivity and electron mobility of bulk structure. Herein, we incorporate TiO2 nanoparticles and Ni(II) sites into a layered cationic imidazolium polymer (IP), in which the imidazolium moieties and free anions can stabilize the key intermediates and enhance the reaction kinetics of CO2 reduction.

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Photocatalytic hydrogen peroxide (HO) generation is largely subject to the sluggish conversion kinetics of the superoxide radical (O) intermediate, which has relatively low reactivity and requires high energy. Here, we present a lattice-strain strategy to accelerate the conversion of O to highly active singlet oxygen(O) by optimizing the distance between two adjacent active sites, thereby stimulating HO generation via low-barrier oxygen-oxygen coupling. As the initial demonstration, the defect-induced strain in ZnInS nanosheet optimizes the distance of two adjacent Zn sites from 3.

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We present an effective strategy for developing the dispersing strong-binding metal In on the surface of weak-binding metal Zn, which modulates the binding energy of the reaction intermediates and further facilitates the efficient conversion of CO to formate. The In-Zn interface (In-Zn2) benefits from the formation of active sites through favorable orbital interactions, leading to a Faradaic efficiency of 82.7% and a formate partial current density of 12.

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The urea oxidation reaction (UOR) has attracted much attention as an efficient alternative reaction to oxygen evolution reaction (OER) due to its low required overpotential. Despite significant progress in efficient nickel-based catalysts, the fundamental issues regarding product selectivity control and dissociation mechanism during the UOR process have not been clarified. Here, we report that tuning the electron delocalization strength of Ni sites significantly affects the OH binding sites, altering urea molecule dissociation patterns in alkaline systems.

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The CO electroreduction reaction has advantages in clean and pollution-free carbon conversion, but it still faces challenges in carbon utilization efficiency and improving the selectivity of C products. Although the dynamic Cu state is known to favor the C-C coupling process, the suitable Cu species for electrocatalytic reduction of CO are difficult to maintain under the conditions of strong reduction and large current. Herein, we propose a Ce doping strategy to stabilize the Cu state (Ce/CuO) during the CORR process, which enables a high Faradaic efficiency of 60 % for multi-carbon products (40 % for CH, 14 % for CHCHOH, and 6 % for CHCOOH), and 25 h stability at -1.

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Solar-driven photocatalytic green hydrogen (H) evolution reaction presents a promising route toward solar-to-chemical fuel conversion. However, its efficiency has been hindered by the desynchronization of fast photogenerated charge carriers and slow surface reaction kinetics. This work introduces a paradigm shift in photocatalyst design by focusing on the synchronization of charge transport and surface reactions through the use of twin structures as a unique platform.

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Multimode responsive optical materials are garnering ever-increasing attention due to their diverse applications. This work showcases a film assembled with rare-earth-doped CaF hollow nanospheres that exhibit water-vapor-triggered dual-mode optical responses. Upon exposure to flowing water vapor, the film rapidly (less than 1.

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Aim: The Barriers to Error Disclosure Assessment (BEDA) tool is used to measure barriers to the disclosure of medical errors by healthcare professionals. This study aimed to evaluate the psychometric properties of the Chinese version of the BEDA (C-BEDA).

Background: The culture of disclosure and transparency in response to medical errors has been recommended in recent years.

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Article Synopsis
  • Researchers have focused on enhancing ion diffusion channels in transition metal oxides for improving ammonium-ion batteries (AIBs) and analyzed how microstructural features affect NH storage and diffusion.
  • By optimizing bond lengths in MnCoO spinel, they found that smaller channel sizes lead to reduced NH adsorption energy and faster hydrogen bond dynamics, facilitating NH movement.
  • The modified MnCoO, combined with oxygen vacancies and carbon nanotubes, showed high specific capacity and impressive cycle stability, resulting in a full cell with excellent energy density and retention after multiple cycles.
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The introduction of noble metal into spinel structure is an effective strategy to develop efficient oxygen evolution/reduction reaction (OER/ORR) catalysts. Herein, surface Co is substituted by Ru in Ru-MnCoO/NCNTs by ion-exchange, where presence of Ru─O─Co unit facilitates electron transfer. This strong electron coupling effect leads downward shift in d-band center and a narrowing of d-p bandgap.

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The photoconversion of CO into valuable chemical products using solar energy is a promising strategy to address both energy and environmental challenges. However, the strongly adsorbed CO frequently impedes the seamless advancement of the subsequent reaction by significantly increasing the reaction activation energy. Here, we present a BiFeO material with lattice strain that collaboratively regulates the d/p-2π* orbitals hybridization between metal sites and *CO as well as *COOH intermediates to achieve rapid conversion of solidly adsorbed CO to critical *COOH intermediates, accelerating the overall CO reduction kinetics.

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A convenient and efficient synthesis of structurally diverse indazolo[1,2-]indazolones a Rh(III)-catalyzed [4 + 1] annulation of 1-arylindazolones with alkynyl cyclobutanols has been achieved by combining C-H and C-C bond cleavage. This cascade reaction features readily available starting materials, good functional group tolerance, broad substrate scope, and excellent atom-economy.

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Given the escalating demand for wearable electronics, there is an urgent need to explore cost-effective and environmentally friendly flexible energy storage devices with exceptional electrochemical properties. However, the existing types of flexible energy storage devices encounter challenges in effectively integrating mechanical and electrochemical performances. This review is intended to provide strategies for the design of components in flexible energy storage devices (electrode materials, gel electrolytes, and separators) with the aim of developing energy storage systems with excellent performance and deformability.

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Hydrogen electrode reactions, including hydrogen evolution reactions and hydrogen oxidation reactions, are fundamental and crucial within aqueous electrochemistry. Particularly in energy-related electrocatalysis processes, there is a consistent involvement of hydrogen-related electrochemical processes, underscoring the need for in-depth study. This review encompasses significant reports, delving into elementary steps and reaction mechanisms of hydrogen electrode reactions, as well as catalyst design strategies.

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Selective photocatalytic reduction of CO to value-added fuels, such as CH, is highly desirable due to its high mass-energy density. Nevertheless, achieving selective CH with higher production yield on p-block materials is hindered by non-ideal adsorption of *CHO key intermediate and an unclear structure-function relationship. Herein, we unlock the key reaction steps of CO and found a volcano-type structure-function relationship for photocatalytic CO-to-CH conversion by gradual reduction of the p-band center of the p-block Bi element leading to formation of Bi-oxygen vacancy heterosites.

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Traditional HO cleavage mediated by macroscopic electron transfer (MET) not only has low utilization of HO, but also sacrifices the stability of catalysts. We present a non-redox hydroxyl-enriched spinel (CuFeO) catalyst with dual Lewis acid sites to realize the homolytic cleavage of HO. The results of systematic experiments, in situ characterizations, and theoretical calculations confirm that tetrahedral Cu sites with optimal Lewis acidity and strong electron delocalization can synergistically elongate the O-O bonds (1.

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Atomically dispersed catalysts are a promising alternative to platinum group metal catalysts for catalyzing the oxygen reduction reaction (ORR), while limited durability during the electrocatalytic process severely restricts their practical application. Here, we report an atomically dispersed Co-doped carbon-nitrogen bilayer catalyst with unique dual-axial Co-C bonds (denoted as Co/DACN) by a smart phenyl-carbon-induced strategy, realizing highly efficient electrocatalytic ORR in both alkaline and acidic media. The corresponding half-wave potential for ORR is up to 0.

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Metal halide perovskites offer ample opportunities to develop advanced optoelectronic devices. This work showcases that the integration of metal halide perovskites into metal oxide nanoshells with controllable interior cavities can enable water-vapor-responsive dual-mode switching of fluorescence and structural color. Through a ship-in-a-bottle method to introduce a controlled amount of CsPbBr into MnO nanoshells, we have designed CsPbBr@MnO yolk-shell nanostructures, which can uptake a defined amount of water to exhibit rapid (less than 1 s) and reversible (≥100 cycles) responses in both fluorescence on-off and color change when exposed to dynamic water vapor.

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Revealing the in-depth structure-property relationship and designing specific capacity electrodes are particularly important for supercapacitors. Despite many efforts made to tune the composition and electronic structure of cobalt oxide for pseudocapacitance, insight into the [CoO] octahedron from the microstructure is still insufficient. Herein, we present a tunable [CoO] octahedron microstructure in LiCoO by a chemical delithiation process.

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To cope with the urgent environmental pressure and tight energy demand, using electrocatalytic methods to drive the reduction of carbon dioxide molecules and produce a variety of fuels and chemicals, is one of the effective pathways to achieve carbon neutrality. In recent years, many significant advances in the study of the electrochemical carbon dioxide reduction reaction (CORR) have been made, but most of the works exhibit low current density, small electrode area and poor long-term stability, which are not suitable for large-scale industrial applications. Herein, combining the research achievements obtained in laboratories and the practical demand of industrial production, we summarize recent frontier progress in the field of the electrochemical CORR, including the fundamentals of catalytic reactions, catalyst design and preparation, and the construction of electrolyzers.

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Breaking the trade-off between activity and selectivity has perennially been a formidable endeavor in the field of hydrogen peroxide (H O ) photosynthesis, especially the side-on configuration of oxygen (O ) on the catalyst surface will cause the cleavage of O-O bonds, which drastically hinders the H O production performance. Herein, we present an atomically heteroatom P doped ZnIn S catalyst with tunable oxygen adsorption configuration to accelerate the ORR kinetics essential for solar-driven H O production. Indeed, the spectroscopy characterizations (such as EXAFS and in situ FTIR) and DFT calculations reveal that heteroatom P doped ZnIn S at substitutional and interstitial sites, which not only optimizes the coordination environment of Zn active sites, but also facilitates electron transfer to the Zn sites and improves charge density, avoiding the breakage of O-O bonds and reducing the energy barriers to H O production.

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Article Synopsis
  • - Zn-based catalysts, particularly undercoordinated Zn sites, show promise in improving CO reduction reactions by optimizing the binding energy of COOH intermediates, potentially replacing noble metal catalysts.
  • - In experiments, Zn/ZnO catalysts exhibit the highest CO selectivity (70.9%) when subjected to specific reduction potentials, and Zn sites were found to effectively suppress competing reactions like hydrogen evolution.
  • - A novel catalyst design featuring a CeO nanotube structure enhances the stability and activity of Zn species, resulting in an impressive faradaic efficiency of 76.9% over 18 hours without significant loss of selectivity.
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Electrocatalytic CO -to-syngas (gaseous mixture of CO and H ) is a promising way to curb excessive CO emission and the greenhouse gas effect. Herein, we present a bimetallic AuZn@ZnO (AuZn/ZnO) catalyst with high efficiency and durability for the electrocatalytic reduction of CO and H O, which enables a high Faradaic efficiency of 66.4 % for CO and 26.

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The sluggish four-electron oxygen evolving reaction is one of the key limitations of photoelectrochemical water decomposition. Optimizing the binding of active sites to oxygen in water and promoting the conversion of *O to *OOH are the key to enhancing oxygen evolution reaction. In this work, W-doped Cu V O (CVO) constructs corner-sharing tetrahedrally coordinated W-V dual active sites to induce the generation of electron deficiency active centers, promote the adsorption of ─OH, and accelerate the transformation of *O to *OOH for water splitting.

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Conducting polymers with high theoretical capacitance and deformability are among the optimal candidates for compressible supercapacitor electrode materials. However, achieving both mechanical and electrochemical stabilities in a single electrode remains a great challenge. To address this issue, the "Polymer Chainmail" is proposed with reversible deformation capability and enhances stability because of the steric hindrance and charge compensation effect of doped anions.

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