Integrated "all-in-one" strategy to construct highly efficient Pd catalyst for CO transformation.

The synthesis of high-value chemicals featuring C-C and/or C-heteroatom bonds CO is critically important, yet efficiently converting thermodynamically stable and kinetically inert linear CO and propargylic amine to the heterocyclic compound 2-oxazolidinone with an integrated catalytic system continues to pose a considerable challenge. Herein, we have designed an "all-in-one" (AIO) palladium (Pd) catalyst (Cat1), distinguished by its co-coordination with acetylglucose (AcGlu) and bis(benzimidazolium) units at the Pd center, which promotes the cyclization of CO and propargylic amine achieving a highest turnover frequency (TOF) of up to 3456 h. Moreover, Cat1 demonstrates excellent stability across various temperatures, with its catalytic activity remaining unchanged even after 10 cycles.

Advanced Architectures of Air Electrodes in Zinc-Air Batteries and Hydrogen Fuel Cells.

The air electrode is an essential component of air-demanding energy storage/conversion devices, such as zinc-air batteries (ZABs) and hydrogen fuel cells (HFCs), which determines the output power and stability of the devices. Despite atom-level modulation in catalyst design being recently achieved, the air electrodes have received much less attention, causing a stagnation in the development of air-demanding equipment. Herein, the evolution of air electrodes for ZABs and HFCs from the early stages to current requirements is reviewed.

Proton-Coupled Electron Transfer Aided Thermoelectric Energy Conversion and Storage.

Low-grade heat is ubiquitous in the environment and its thermoelectric conversion by the ionic conductors remains a challenge because of the low efficiency and poor sustainability. Here we demonstrate that the thermoelectric performances can be boosted by combining the Soret effect of protons and proton-coupled electron transfer (PCET) reaction of benzoquinone and hydroquinone in hydrogels. An overall enhancement of thermopower (25.

Electron-Donors-Acceptors Interaction Enhancing Electrocatalytic Activity of Metal-Organic Polymers for Oxygen Reduction.

Catalysts with metal-N sites have long been considered as effective electrocatalysts for oxygen reduction reaction (ORR), yet the accurate structure-property correlations of these active sites remain debatable. Report here is a proof-of-concept method to construct 1,4,8,11-tetraaza[14]annulene (TAA)-based polymer nanocomposites with well-managed electronic microenvironment via electron-donors/acceptors interaction of altering electron-withdrawing β-site substituents. DFT calculation proves the optimal -Cl substituted catalyst (CoTAA-Cl@GR) tailored the key OH* intermediate interaction with Co-N sites under the d-orbital regulation, hence reaching the top of ORR performance with excellent turnover frequency (0.

Longitudinally Grafting of Graphene with Iron Phthalocyanine-based Porous Organic Polymer to Boost Oxygen Electroreduction.

Iron phthalocyanine-based polymers (PFePc) are attractive noble-metal-free candidates for catalyzing oxygen reduction reaction (ORR). However, the low site-exposure degree and poor electrical conductivity of bulk PFePc restricted their practical applications. Herein, laminar PFePc nanosheets covalently and longitudinally linked to graphene (3D-G-PFePc) was prepared.

Solute-solvent dual engineering toward versatile electrolyte for high-voltage aqueous zinc-based energy storage devices.

Manufacturing cost-effective electrolytes featuring high (electro)chemical stability, high Zn anode reversibility, good ionic conductivity, and environmental benignity is highly desired for rechargeable aqueous zinc-based energy storage devices but remains a great challenge. Herein, a solute-solvent dual engineering strategy using lithium bis(trifluoromethane)sulfonimide (LiTFSI) and inexpensive poly(ethylene glycol) (PEG, = 200) as a coadditive with an optimized ratio accomplished an all-round performance enhancement of electrolytes. Due to the synergistic inhibition of water activity and Zn solvation structure reorganization by LiTFSI-PEG, as well as a stable F-rich interfacial layer and PEG adsorption on the Zn anode surface, dendrite-free Zn plating/stripping at nearly 100% Coulombic efficiency and stable cycling performance over 2000 h at 0.

Fine-Tuning BiTe-Copper Selenide Alloys Enables an Efficient n-Type Thermoelectric Conversion.

Bismuth tellurides is one of the most promising thermoelectric (TE) material candidates in low-temperature application circumstances, but the n-type thermoelectric property is relatively low compared to the p-type counterpart and still needs to be improved. Herein, we incorporated different copper selenides (CuSe, CuSe and CuSe) into a BiTe matrix to create the alloy by grinding and successive sintering to enable higher thermoelectric performance. The results demonstrated that all alloys achieved n-type TE characteristics and BiTe-CuSe exhibited the best Seebeck coefficient and power factor among them.

Understanding the electrocatalytic mechanism of self-template formation of hierarchical CoS/NiS heterojunctions for highly selective electroreduction of nitrobenzene.

Aqueous electrochemical nitroarene reduction reaction using HO as the sustainable hydrogen source is an emerging technology to produce functionalized anilines. However, the development of low-cost electrocatalysts and the fundamental mechanistic understanding of the selective NO-RR still remain challenging. Herein, self-supporting hierarchical nanosheets consisting of high-density CoS/NiS heterojunctions on Ni foam (CoS/NiS-NF) are constructed an self-template strategy.

Facile synthesis of copper selenides with different stoichiometric compositions and their thermoelectric performance at a low temperature range.

Copper selenide is widely considered to be a promising candidate for high-performance flexible thermoelectrics; however, most of the reported values of copper selenides are unsatisfactory at a relatively low temperature range. Herein, we utilized some wet chemical methods to synthesize a series of copper selenides. XRD, SEM and TEM characterizations revealed that CuSe, CuSe and Cu Se were prepared successfully and possessed different morphologies and sizes.

Simultaneously Integrate Iron Single Atom and Nanocluster Triggered Tandem Effect for Boosting Oxygen Electroreduction.

Atomically nitrogen-coordinated iron atoms on carbon (FeNC) catalysts are emerging as attractive materials to substitute precious-metal-based catalysts for the oxygen reduction reaction (ORR). However, FeNC usually suffers from unsatisfactory performance due to the symmetrical charge distribution around the iron site. Elaborately regulating the microenvironment of the central Fe atom can substantially improve the catalytic activity of FeNC, which remains challenging.

High Energy and Power Zinc Ion Capacitors: A Dual-Ion Adsorption and Reversible Chemical Adsorption Coupling Mechanism.

Zinc ion capacitors (ZICs) hold great promise in large-scale energy storage by inheriting the superiorities of zinc ion batteries and supercapacitors. However, the mismatch of kinetics and capacity between a Zn anode and a capacitive-type cathode is still the Achilles' heel of this technology. Herein, porous carbons are fabricated by using tetra-alkali metal pyromellitic acid salts as precursors through a carbonization/self-activation procedure for enhancing zinc ion storage.

Deciphering the Precursor-Performance Relationship of Single-Atom Iron Oxygen Electroreduction Catalysts via Isomer Engineering.

Single atom Fe-nitrogen-carbon (Fe-N-C) catalysts have high catalytic activity and selectivity for the oxygen reduction reaction (ORR), and are possible alternatives for Pt-based materials. However, the reasonable design and selection of precursors to establish their relationship with Fe-N-C catalyst performance is still a formidable task. Herein, precursors with controllable structures are easily achieved through isomer engineering, with the purpose of regulating the active site density and microscopic morphology of the final electrocatalyst.

Optimizing Microenvironment of Asymmetric N,S-Coordinated Single-Atom Fe via Axial Fifth Coordination toward Efficient Oxygen Electroreduction.

Single-atom catalysts (SACs) are attractive candidates for oxygen reduction reaction (ORR). The catalytic performances of SACs are mainly determined by the surrounding microenvironment of single metal sites. Microenvironment engineering of SACs and understanding of the structure-activity relationship is critical, which remains challenging.

Fast assembly of MXene hydrogels by interfacial electrostatic interaction for supercapacitors.

A simple and fast method for preparing MXene hydrogels is proposed by introducing protonated thionine molecules into a MXene dispersion through electrostatic interaction. Such a 3D hydrogel effectively suppressed restacking and oxidation, and enlarged the surface utilization of the MXene, producing an improved specific capacitance of 163 F g at 1 A g and excellent stability when used as an electrode material for supercapacitors.

Simultaneously Integrating Single Atomic Cobalt Sites and Co S Nanoparticles into Hollow Carbon Nanotubes as Trifunctional Electrocatalysts for Zn-Air Batteries to Drive Water Splitting.

The development of rechargeable metal-air batteries and water electrolyzers are highly constrained by electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). However, the construction of efficient trifunctional electrocatalysts for ORR/OER/HER are highly desirable yet challenging. Herein, hollow carbon nanotubes integrated single cobalt atoms with Co S nanoparticles (CoSA + Co S /HCNT) are fabricated by a straightforward in situ self-sacrificing strategy.

Boosting Oxygen Reduction of Single Iron Active Sites via Geometric and Electronic Engineering: Nitrogen and Phosphorus Dual Coordination.

Atomically dispersed transition metal active sites have emerged as one of the most important fields of study because they display promising performance in catalysis and have the potential to serve as ideal models for fundamental understanding. However, both the preparation and determination of such active sites remain a challenge. The structural engineering of carbon- and nitrogen-coordinated metal sites (M-N-C, M = Fe, Co, Ni, Mn, Cu, etc.

CoO Supraparticle-Based Bubble Nanofiber and Bubble Nanosheet with Remarkable Electrochemical Performance.

Hollow nanostructures based on transition metal oxides (TMOs) with high surface-to-volumetric ratio, low density, and high loading capacity have received great attention for energy-related applications. However, the controllable fabrication of hybrid TMO-based hollow nanostructures in a simple and scalable manner remains challenging. Herein, a simple and scalable strategy is used to prepare hierarchical carbon nanofiber (CNF)-based bubble-nanofiber-structured and reduced graphene oxide (RGO)-based bubble-nanosheet-structured CoO hollow supraparticle (HSP) composites (denoted as CNF/HSP-CoO and RGO/HSP-CoO, respectively) by solution self-assembly of ultrasmall CoO nanoparticles (NPs) assisting with polydopamine (PDA) modification.

FeO-Encapsulating N-doped porous carbon materials as efficient oxygen reduction reaction electrocatalysts for Zn-air batteries.

FeO nanoparticle-encapsulating N-doped porous carbon was synthesized. Owing to the large specific surface area, hierarchical porous structure, and sufficient number of active sites from the graphitic carbon wrapped FeO NPs as well as the joint effect with Fe-N moieties, the as-prepared 2D-FeO@FeNC-700 electrocatalyst exhibits exceptional performance in Zn-air batteries.

Three-dimensional TiO2/ZnO hybrid array as a heterostructured anode for efficient quantum-dot-sensitized solar cells.

The development of a novel nanoarray photoanode with a heterostructure on a transparent conducting oxide substrate provides a promising scheme to fabricate efficient energy conversion devices. Herein, we successfully synthesize the vertically aligned hierarchical TiO2 nanowire/ZnO nanorod or TiO2 nanowire/ZnO nanosheet hybrid arrays, which are proven to be excellent anode candidates for superior light utilization. Consequently, the quantum-dot-sensitized solar cells based on such hybrid arrays exhibit an impressive power conversion efficiency (PCE) under AM 1.

Hierarchical macroporous Zn(2)SnO(4)-ZnO nanorod composite photoelectrodes for efficient CdS/CdSe quantum dot co-sensitized solar cells.

A hierarchical macroporous Zn2SnO4-ZnO nanorod composite film is prepared through a drop-casting process of PS@Zn2SnO4 and subsequent hydrothermal growth of ZnO nanorod. CdS/CdSe co-sensitized solar cells based on the macroporous Zn2SnO4-ZnO nanorod composite photoelectrode exhibits an enhancement of 34.4% in power conversion efficiency (1.