Ammonia (NH) is vital in global production and energy cycles. Electrocatalytic nitrate reduction (e-NORR) offers a promising route for nitrogen (N) conversion and NH synthesis, yet it faces challenges like competing reactions and low catalyst activity. This study proposes a synergistic mechanism incorporating a proton donor to mediate O-end e-NORR, addressing these limitations.
View Article and Find Full Text PDFPrussian blue analogs (PBAs), as a classical kind of microporous materials, have attracted substantial interests considering their well-defined framework structures, unique physicochemical properties and low cost. However, PBAs typically adopt cubic structure that features small pore size and low specific surface area, which greatly limits their practical applications in various fields ranging from gas adsorption/separation to energy conversion/storage and biomedical treatments. Here we report the facile and general synthesis of unconventional hexagonal open PBA structures.
View Article and Find Full Text PDFCurrently, there are still obstacles to rationally designing the ligand fields to activate rare-earth (RE) elements with satisfactory intrinsic electrocatalytic reactivity. Herein, axial coordination strategies and nanostructure design are applied for the construction of La single atoms (La-Cl SAs/NHPC) with satisfactory oxygen reduction reaction (ORR) activity. The nontrivial LaNCl motifs configuration and the hierarchical porous carbon substrate that facilitates maximized metal atom utilization ensure high half-wave potential (0.
View Article and Find Full Text PDFMetallic 1T phase molybdenum disulfide (MoS) is among the most promising electrode materials for supercapacitors, but its capacitance and cyclability remain to be improved to meet the constantly increasing energy storage needs in portable electronics. In this study, we present a strategy, covalent functionalization, which achieves the improvement of capacitance of metallic 1T phase MoS. Covalently functionalized by the modifier 4-bromobenzenediazonium tetrafluoroborate, the metallic MoS membrane exhibits increased interlayer spacing, slightly curled layered architecture, enhanced charge transfer, and improved adsorption capabilities toward electrolyte molecules and ions.
View Article and Find Full Text PDFThe development of efficient and durable electrocatalysts for the acidic oxygen evolution reaction (OER) is essential for advancing renewable hydrogen energy technology. However, the slow deprotonation kinetics of oxo-intermediates, involving the four proton-coupled electron steps, hinder the acidic OER progress. Herein, a RuTiO solid solution electrocatalyst is investigated, which features bridged oxygen (O) sites that act as proton acceptors, accelerating the deprotonation of oxo-intermediates.
View Article and Find Full Text PDFElectrochemical nitrate reduction reaction (NORR) is emerging as a promising strategy for nitrate removal and ammonia (NH) production using renewable electricity. Although great progresses have been achieved, the crystal phase effect of electrocatalysts on NORR remains rarely explored. Here, the epitaxial growth of unconventional 2H Cu on hexagonal close-packed (hcp) IrNi template, resulting in the formation of three IrNiCu@Cu nanostructures, is reported.
View Article and Find Full Text PDFPersistent luminescence describes the phenomenon whereby luminescence remains after the stoppage of excitation. Recently, upconversion persistent luminescence (UCPL) phosphors that can be directly charged by near-infrared (NIR) light have gained considerable attention due to their promising applications ranging from photonics to biomedicine. However, current lanthanide-based UCPL phosphors show small absorption cross sections and low upconversion charging efficiency.
View Article and Find Full Text PDFThe synthesis of nitrate by the electrochemical N oxidation reaction (NOR) is currently one of the most promising routes. However, the traditional generation of nitrate depends on the oxidation reaction between N and HO (or ·OH), which involves complex reaction steps and intermediates, showing strong competition from oxygen evolution reaction (OER). Here, an effective NOR method is proposed to directly oxidize N by using O as a reactive oxygen source to reduce the reaction step.
View Article and Find Full Text PDFManipulating the crystallographic orientation of zinc deposition is recognized as an effective approach to address zinc dendrites and side reactions for aqueous zinc-ion batteries (ZIBs). We introduce 2-methylimidazole (Mlz) additive in zinc sulfate (ZSO) electrolyte to achieve vertical electrodeposition with preferential orientation of the (100) and (110) crystal planes. Significantly, the zinc anode exhibited long lifespan with 1500 h endurance at 1 mA cm and an excellent 400 h capability at a depth of discharge (DOD) of 34% in Zn||Zn battery configurations, while in Zn||MnO battery assemblies, a capacity retention of 68.
View Article and Find Full Text PDFLiquid-solid contact electrification (CE) is essential to diverse applications. Exploiting its full implementation requires an in-depth understanding and fine-grained control of charge carriers (electrons and/or ions) during CE. Here, we decouple the electrons and ions during liquid-solid CE by designing binary superhydrophobic surfaces that eliminate liquid and ion residues on the surfaces and simultaneously enable us to regulate surface properties, namely work function, to control electron transfers.
View Article and Find Full Text PDFCopper (Cu) nanomaterials are a unique kind of electrocatalysts for high-value multi-carbon production in carbon dioxide reduction reaction (CORR), which holds enormous potential in attaining carbon neutrality. However, phase engineering of Cu nanomaterials remains challenging, especially for the construction of unconventional phase Cu-based asymmetric heteronanostructures. Here the site-selective growth of Cu on unusual phase gold (Au) nanorods, obtaining three kinds of heterophase fcc-2H-fcc Au-Cu heteronanostructures is reported.
View Article and Find Full Text PDFTwo-electron oxygen reduction reaction (2e ORR) is of great significance to HO production and reversible nonalkaline Zn-air batteries (ZABs). Multiple oxygen-containing sp-bonded nanocarbons have been developed as electrocatalysts for 2e ORR, but they still suffer from poor activity and stability due to the limited and mixed active sites at the edges as well as hydrophilic character. Herein, graphdiyne (GDY) with rich sp-C bonds is studied for enhanced 2e ORR.
View Article and Find Full Text PDFThe controlled synthesis of metal nanomaterials with unconventional phases is of significant importance to develop high-performance catalysts for various applications. However, it remains challenging to modulate the atomic arrangements of metal nanomaterials, especially the alloy nanostructures that involve different metals with distinct redox potentials. Here we report the general one-pot synthesis of IrNi, IrRhNi and IrFeNi alloy nanobranches with unconventional hexagonal close-packed (hcp) phase.
View Article and Find Full Text PDFThe manipulation of excitation modes and resultant emission colors in luminescent materials holds pivotal importance for encrypting information in anti-counterfeiting applications. Despite considerable achievements in multimodal and multicolor luminescent materials, existing options generally suffer from static monocolor emission under fixed external stimulation, rendering them vulnerability to replication. Achieving dynamic multimodal luminescence within a single material presents a promising yet challenging solution.
View Article and Find Full Text PDFWith the merits of the high energy density of batteries and power density of supercapacitors, the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required. However, the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan. It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors.
View Article and Find Full Text PDFThe development of efficient and stable catalysts for hydrogen production from electrolytic water in a wide pH range is of great significance in alleviating the energy crisis. Herein, Pt nanoparticles (NPs) anchored on the vacancy of high entropy rare earth oxides (HEREOs) were prepared for the first time for highly efficient hydrogen production by water electrolysis. The prepared Pt-(LaCeSmYErGdYb)O showed excellent electrochemical performances, which require only 12, 57, and 77 mV to achieve a current density of 100 mA cm in 0.
View Article and Find Full Text PDFReaching rapid reaction kinetics of oxygen reduction (ORR) and oxygen evolution reactions (OER) is critical for realizing efficient rechargeable zinc-air batteries (ZABs). Herein, a novel CoNi-CoN composite site containing CoNi alloyed nanoparticles and CoN moieties is first constructed in N-doped carbon nanosheet matrix (CoNi-CoN/C). Benefiting from the high electroactivity of CoNi-CoN composite sites and large surface area, CoNi-CoN/C shows a superior half-wave potential (0.
View Article and Find Full Text PDFElectrocatalytic carbon dioxide reduction reaction (CORR) toward value-added chemicals/fuels has offered a sustainable strategy to achieve a carbon-neutral energy cycle. However, it remains a great challenge to controllably and precisely regulate the coordination environment of active sites in catalysts for efficient generation of targeted products, especially the multicarbon (C) products. Herein we report the coordination environment engineering of metal centers in coordination polymers for efficient electroreduction of CO to C products under neutral conditions.
View Article and Find Full Text PDFBimetallic PtRu are promising electrocatalysts for hydrogen oxidation reaction in anion exchange membrane fuel cell, where the activity and stability are still unsatisfying. Here, PtRu nanowires were implanted with a series of oxophilic metal atoms (named as i-M-PR), significantly enhancing alkaline hydrogen oxidation reaction (HOR) activity and stability. With the dual doping of In and Zn atoms, the i-ZnIn-PR/C shows mass activity of 10.
View Article and Find Full Text PDFElectrocatalytic nitrate reduction reaction (NORR) toward ammonia synthesis is recognized as a sustainable strategy to balance the global nitrogen cycle. However, it still remains a great challenge to achieve highly efficient ammonia production due to the complex proton-coupled electron transfer process in NORR. Here, the controlled synthesis of RuMo alloy nanoflowers (NFs) with unconventional face-centered cubic (fcc) phase and hexagonal close-packed/fcc heterophase for highly efficient NORR is reported.
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