Defect-Engineered Nanozyme-Linked Receptors.

Though nanozymes are successfully applied in various areas, the increasing demands facilitate the exploitation of nanozymes possessing higher activity and more functions. Natural enzyme-linked receptors (ELRs) are critical components for signal transductions in vivo by expressing activity variations after binding with ligands. Inspired by this, the defect-engineered carbon nitrides (DCN) are reported to serve as nanozyme-linked receptors (NLRs).

Two-Dimensional-Plasmon-Boosted Iron Single-Atom Electrochemiluminescence for the Ultrasensitive Detection of Dopamine, Hemin, and Mercury.

Single-atom catalysts (SACs) have recently been exploited for luminol-dissolved oxygen electrochemiluminescence (ECL); however, they still suffer from low sensitivity and narrow detection range for a real sample assay. In this work, we boost markedly the ECL response of the iron SAC (Fe-SAC)-based system, for the first time, by the excitation of two-dimensional plasmons derived from the Au@SiO nanomembrane. The plausible mechanism of plasmon enhancement in the Fe-SAC ECL system has been discussed.

An Adjacent Atomic Platinum Site Enables Single-Atom Iron with High Oxygen Reduction Reaction Performance.

The modulation effect has been widely investigated to tune the electronic state of single-atomic M-N-C catalysts to enhance the activity of oxygen reduction reaction (ORR). However, the in-depth study of modulation effect is rarely reported for the isolated dual-atomic metal sites. Now, the catalytic activities of Fe-N moiety can be enhanced by the adjacent Pt-N moiety through the modulation effect, in which the Pt-N acts as the modulator to tune the 3d electronic orbitals of Fe-N active site and optimize ORR activity.

Effect of three-dimensional conformal radiotherapy and intensity-modulated radiotherapy on parotid gland function and quality of life in patients with nasopharyngeal carcinoma.

Objective: To investigate the effects of three-dimensional conformal radiotherapy (3DCRT) and intensity-modulated radiotherapy (IMRT) on parotid gland function and quality of life in patients with nasopharyngeal carcinoma (NPC).

Methods: Ninety-six patients with NPC diagnosed and treated in our hospital were divided into two groups using a random number table. The control group was treated with three-dimensional conformal radiotherapy and the research group was treated with intensity-modulated radiotherapy.

Atomically Dispersed Pt-NC Sites Enabling Efficient and Selective Electrocatalytic C-C Bond Cleavage in Lignin Models under Ambient Conditions.

Selective cleavage of C-C linkages is the key and a challenge for lignin degradation to harvest value-added aromatic compounds. To this end, electrocatalytic oxidation presents a promising technique by virtue of mild reaction conditions and strong sustainability. However, the existing electrocatalysts (traditional bulk metal and metal oxides) for C-C bond oxidative cleavage suffer from poor selectivity and low product yields.

Atomically Dispersed Fe-N Modified with Precisely Located S for Highly Efficient Oxygen Reduction.

Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-substrate interaction. Herein, atomically dispersed Fe-NC material with precise sulfur modification to Fe periphery (termed as Fe-NSC) was synthesized, X-ray absorption near edge structure analysis confirmed the central Fe atom being stabilized in a specific configuration of Fe(N)(N-C-S). By enabling precisely localized S doping, the electronic structure of Fe-N moiety could be mediated, leading to the beneficial adjustment of absorption/desorption properties of reactant/intermediate on Fe center.

Competitive Coordination of Chloride and Fluoride Anions Towards Trivalent Lanthanide Cations (La and Nd ) in Molten Salts.

Molten salt electrolysis is a vital technique to produce high-purity lanthanide metals and alloys. However, the coordination environments of lanthanides in molten salts, which heavily affect the related redox potential and electrochemical properties, have not been well elucidated. Here, the competitive coordination of chloride and fluoride anions towards lanthanide cations (La and Nd ) is explored in molten LiCl-KCl-LiF-LnCl salts using electrochemical, spectroscopic, and computational approaches.

Modulating Oxygen Reduction Behaviors on Nickel Single-Atom Catalysts to Probe the Electrochemiluminescence Mechanism at the Atomic Level.

Luminol-dissolved O electrochemiluminescence (ECL)-sensing platforms have been widely developed for sensitive and reliable detection, while their actual ECL mechanisms are still in controversy due to the involved multiple reactive oxygen species (ROS). Different from the structural complexity of nanomaterials, well-defined single-atom catalysts (SACs) as coreaction accelerators will provide great prospects for investigating the ECL mechanism at the atomic level. Herein, two carbon-supported nickel SACs with the active centers of Ni-N (Ni-N/C) and Ni-NO (Ni-NO/C) were synthesized as efficient coreaction accelerators to enhance the ECL signals of a luminol-dissolved O system.

Grey hematite photoanodes decrease the onset potential in photoelectrochemical water oxidation.

Photoelectrochemical (PEC) water splitting for solar energy conversion into chemical fuels has attracted intense research attention. The semiconductor hematite (α-FeO), with its earth abundance, chemical stability, and efficient light harvesting, stands out as a promising photoanode material. Unfortunately, its electron affinity is too deep for overall water splitting, requiring additional bias.

Boosting CO Electroreduction via the Synergistic Effect of Tuning Cationic Clusters and Visible-Light Irradiation.

Introducing an external light field can increase the intrinsic activity and energy efficiency for electrochemical CO reduction. Herein, a synergistic strategy that introduces photosensitive components and visible light into a stable system is reported to improve the performance for CO reduction. The catalytic kinetics studies indicate that the synergistic effect of implantation of cationic Ti and additional light driving is the primary responsibility for accelerating the first electron transfer to form a *COO intermediate.

Copper single-atom catalysts with photothermal performance and enhanced nanozyme activity for bacteria-infected wound therapy.

Nanozymes have become a new generation of antibiotics with exciting broad-spectrum antibacterial properties and negligible biological toxicity. However, their inherent low catalytic activity limits their antibacterial properties. Herein, Cu single-atom sites/N doped porous carbon (Cu SASs/NPC) is successfully constructed for photothermal-catalytic antibacterial treatment by a pyrolysis-etching-adsorption-pyrolysis (PEAP) strategy.

Synthesis of a Boron-Imidazolate Framework Nanosheet with Dimer Copper Units for CO Electroreduction to Ethylene.

Fundamental understanding of the dependence between the structure and composition on the electrochemical CO reduction reaction (CO RR) would guide the rational design of highly efficient and selective electrocatalysts. A major impediment to the deep reduction CO to multi-carbon products is the complexity of carbon-carbon bond coupling. The chemically well-defined catalysts with atomically dispersed dual-metal sites are required for these C-C coupling involved processes.

Ternary nickel-tungsten-copper alloy rivals platinum for catalyzing alkaline hydrogen oxidation.

Operating fuel cells in alkaline environments permits the use of platinum-group-metal-free (PGM-free) catalysts and inexpensive bipolar plates, leading to significant cost reduction. Of the PGM-free catalysts explored, however, only a few nickel-based materials are active for catalyzing the hydrogen oxidation reaction (HOR) in alkali; moreover, these catalysts deactivate rapidly at high anode potentials owing to nickel hydroxide formation. Here we describe that a nickel-tungsten-copper (NiWCu) ternary alloy showing HOR activity rivals Pt/C benchmark in alkaline electrolyte.

Interface-Promoted Direct Oxidation of -Arsanilic Acid and Removal of Total Arsenic by the Coupling of Peroxymonosulfate and Mn-Fe-Mixed Oxide.

As one of the extensively used feed additives in livestock and poultry breeding, -arsanilic acid (-ASA) has become an organoarsenic pollutant with great concern. For the efficient removal of -ASA from water, the combination of chemical oxidation and adsorption is recognized as a promising process. Herein, hollow/porous Mn-Fe-mixed oxide (MnFeO) nanocubes were synthesized and used in coupling with peroxymonosulfate (PMS) to oxidize -ASA and remove the total arsenic (As).

Direct Observation of Metal Oxide Nanoparticles Being Transformed into Metal Single Atoms with Oxygen-Coordinated Structure and High-Loadings.

Direct conversion of bulk metal or nanoparticles into metal single atoms under thermal pyrolysis conditions is a highly efficient and promising strategy to fabricate single-atom catalysts (SACs). Usually, nitrogen-doped carbon is used as the anchoring substrate to capture the migrating metal ion species at high temperatures, and stable isolated SACs with nitrogen coordination are formed during the process. Herein, we report unexpected oxygen-coordinated metal single-atom catalysts (Fe-, Co-, Ni-, Mn-SACs) with high loadings (above 10 wt %) through direct transformation of metal oxide nanoparticles (Fe-, Co-, Ni-, Mn-NPs) in an inert atmosphere at 750 °C for 2 h.

Highly Active Heterogeneous Catalyst for Ethylene Dimerization Prepared by Selectively Doping Ni on the Surface of a Zeolitic Imidazolate Framework.

The production of 1-butene by ethylene dimerization is an important chemical industrial process currently implemented using homogeneous catalysts. Here, we describe a highly active heterogeneous catalyst (Ni-ZIF-8) for ethylene dimerization, which consists of isolating Ni-active sites selectively located on the crystal surface of a zeolitic imidazolate framework. Ni-ZIF-8 can be easily prepared by a simple one-pot synthesis method in which site-specific anchoring of Ni is achieved spontaneously because of the incompatibility between the d electronic configuration of Ni and the three-dimensional framework of ZIF-8.

Subsurface-Regulated PtGa Nanoparticles Confined in Silicalite-1 for Propane Dehydrogenation.

Propane dehydrogenation (PDH) is one of the most promising techniques to produce propylene. Industrial Pt-based catalysts often suffer from short-time stability under high temperature due to serious sintering and coke deposition via undesired side reactions. Detailed reaction mechanism on the surface of Pt-based nanoparticle has been well studied, while the subsurface effect remains mostly unstudied.

Anomalous self-optimization of sulfate ions for boosted oxygen evolution reaction.

Broadly, the oxygen evolution reaction (OER) has been deeply understood as a significant part of energy conversion and storage. Nevertheless, the anions in the OER catalysts have been neglected for various reasons such as inactive sites, dissolution, and oxidation, amongst others. Herein, we applied a model catalyst s-Ni(OH) to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.

FeC-Assisted Single Atomic Fe Sites for Sensitive Electrochemical Biosensing.

The rational construction of advanced sensing platforms to sensitively detect HO produced by living cells is one of the challenges in both physiological and pathological fields. Owing to the extraordinary catalytic performances and similar metal coordination to natural metalloenzymes, single atomic site catalysts (SASCs) with intrinsic peroxidase (POD)-like activity have shown great promise for HO detection. However, there still exists an obvious gap between them and natural enzymes because of the great challenge in rationally modulating the electronic and geometrical structures of central atoms.

Tuning Co Coordination in Cobalt Layered Double Hydroxide Nanosheets via Fe Doping for Efficient Oxygen Evolution.

Inexpensive and efficient electrocatalysts are crucial for the development and practical application of energy conversion and storage technologies. Layered-double-hydroxide (LDH) materials have attracted much attention due to the special layered structure, but their electrocatalytic activity and stability are still limited. Herein, we propose to tune Co occupancy and coordination in cobalt-based LDH nanosheets via Fe doping for efficient and stable electrocatalysis for oxygen evolution reaction (OER).

Highly Efficient NO Abatement over Cu-ZSM-5 with Special Nanosheet Features.

Conventional Cu-ZSM-5 and special Cu-ZSM-5 catalysts with diverse morphologies (nanoparticles, nanosheets, hollow spheres) were synthesized and comparatively investigated for their performances in the selective catalytic reduction (SCR) of NO to N with ammonia. Significant differences in SCR behavior were observed, and nanosheet-like Cu-ZSM-5 showed the best SCR performance with the lowest of 130 °C and nearly complete conversion in the temperature range of 200-400 °C. It was found that Cu-ZSM-5 nanosheets [mainly exposed (0 1 0) crystal plane] with abundant mesopores and framework Al species were favorable for the formation of high external surface areas and Al pairs, which influenced the local environment of Cu.

Peroxo Species Formed in the Bulk of Silicate Cathodes.

Oxygen redox in Li-rich oxides may boost the energy density of lithium-ion batteries by incorporating oxygen chemistry in solid cathodes. However, oxygen redox in the bulk usually entangles with voltage hysteresis and oxygen release, resulting in a prolonged controversy in literature on oxygen transformation. Here, we report spectroscopic evidence of peroxo species formed and confined in silicate cathodes amid oxygen redox at high voltage, accompanied by Co /Co redox dominant at low voltage.

A novel Fe/N/C electrocatalyst prepared from a carbon-supported iron(ii) complex of macrocyclic ligands for oxygen reduction reaction.

Herein, we report a novel method to synthesize Fe/N/C composites from a carbon-supported iron (ii) coordination complex of 2,3-dicyanotetraazabenzotriphenylene (2,3-DCTBT) ligands towards oxygen reduction reaction (ORR) in alkaline media. We investigated the influence of different temperatures during the thermal carbonization process on the performance of the catalyst, and Fe/N/C-900 stood out among all other samples because of the existence of Fe-N active sites. The as-obtained Fe/N/C-900 exhibited excellent electrochemical performance ( is 0.

Magnetic-Field-Stimulated Efficient Photocatalytic N Fixation over Defective BaTiO Perovskites.

Efficient coupling solar energy conversion and N fixation by photocatalysis has been shown promising potentials. However, the unsatisfied yield rate of NH curbs its forward application. Defective typical perovskite, BaTiO , shows remarkable activity under an applied magnetic field for photocatalytic N fixation with an NH yield rate exceeding 1.