Coordination Environment Engineering to Regulate the Adsorption Strength of Intermediates in Single Atom Catalysts for High-performance CO Reaction Reduction.

The modulation of the coordination environment of single atom catalysts (SACs) plays a vital role in promoting CO reduction reaction (CORR). Herein, N or B doped Fe-embedded graphyne (Fe-GY), Fe-nXGYm (n = 1, 2, 3; X = N, B; m = 1, 2, 3), are employed as probes to reveal the effect of the coordination environment engineering on CORR performance via heteroatom doping in SACs. The results show that the doping position and number of N or B in Fe-GY significantly affects catalyst activity and CORR product selectivity.

Eco-Friendly Cerium-Cobalt Counter-Doped BiSe Nanoparticulate Semiconductor: Synergistic Doping Effect for Enhanced Thermoelectric Generation.

Metal chalcogenides are primarily used for thermoelectric applications due to their enormous potential to convert waste heat into valuable energy. Several studies focused on single or dual aliovalent doping techniques to enhance thermoelectric properties in semiconductor materials; however, these dopants enhance one property while deteriorating others due to the interdependency of these properties or may render the host material toxic. Therefore, a strategic doping approach is vital to harness the full potential of doping to improve the efficiency of thermoelectric generation while restoring the base material eco-friendly.

Enhanced CO capture in partially interpenetrated MOFs: Synergistic effects from functional group, pore size, and steric-hindrance.

Excessive CO emissions have contributed to global environmental issues, driving the development of CO capture adsorbents. Among various candidates, metal-organic frameworks (MOFs) are considered the most promising due to their unique microporous structure. Herein, a series of partially interpenetrated MOFs named UPC-XX were built to investigate the continuous enhancement in CO capture performance via synergistic effects from functional group, pore size, and steric-hindrance using theoretical calculations.

Role of transition metal d-orbitals in single-atom catalysts for nitric oxide electroreduction to ammonia.

Recently, surging interests exist in direct electrochemical ammonia (NH) synthesis from nitric oxide (NO) due to the dual benefit of NH synthesis and NO removal. However, designing highly efficient catalysts is still challenging. Based on density functional theory, the best ten candidates of transition-metal atoms (TMs) embedded in phosphorus carbide (PC) monolayer is screened out as highly active catalysts for direct NO-to-NH electroreduction.

Inducing Fe 3d Electron Delocalization and Spin-State Transition of FeN Species Boosts Oxygen Reduction Reaction for Wearable Zinc-Air Battery.

Transition metal-nitrogen-carbon materials (M-N-Cs), particularly Fe-N-Cs, have been found to be electroactive for accelerating oxygen reduction reaction (ORR) kinetics. Although substantial efforts have been devoted to design Fe-N-Cs with increased active species content, surface area, and electronic conductivity, their performance is still far from satisfactory. Hitherto, there is limited research about regulation on the electronic spin states of Fe centers for Fe-N-Cs electrocatalysts to improve their catalytic performance.

Can Charge-Modulated Metal-Organic Frameworks Achieve High-Performance CO Capture and Separation over H , N , and CH ?

CO capture and separation by using charge-modulated adsorbent materials is a promising strategy to reduce CO emissions. Herein, three TM-HAB (TM=Co, Ni, and Cu; HAB=hexa-aminobenzene) metal-organic frameworks (MOFs) were evaluated as charge-modulated CO capture and separation materials by using density functional theory and grand canonical Monte Carlo simulations. The results showed that each TM-HAB presented a high electrical conductivity and structural stability when injecting charges.

Surface Engineering of Flower-Like Ionic Liquid-Functionalized Graphene Anchoring Palladium Nanocrystals for a Boosted Ethanol Oxidation Reaction.

The development of low-cost and high-performance electrocatalyst-supporting materials is desirable and necessary for the ethanol oxidation reaction (EOR). Here, we report a facile and universal template-free approach for the first time to synthesize three-dimensional (3D) flower-like ionic liquid-functionalized graphene (IL-RGO). Then, the crystalline Pd nanoparticles were anchored on IL-RGO by a simple wet chemical growth method without a surfactant (denoted as Pd/IL-RGO).

In vivo liquid biopsy for glioblastoma malignancy by the AFM and LSPR based sensing of exosomal CD44 and CD133 in a mouse model.

Glioblastoma (GBM) is the fatal brain tumor in which secreted lactate enhances the expression of cluster of differentiation 44 (CD44) and the release of exosomes, cell-derived nanovesicles (30-200 nm), and therefore promotes tumor malignant progression. This study found that lactate-driven upregulated CD44 in malignant Glioblastoma cells (GMs) enhanced the release of CD44-enriched exosomes which increased GMs' migration and endothelial cells' tube formation, and CD44 in the secreted exosomes was sensitively detected by "capture and sensing" Titanium Nitride (TiN) - Nanoholes (NH) - discs immunocapture (TIC) - atomic force microscopy (AFM) and ultrasensitive TiN-NH-localized surface plasmon resonance (LSPR) biosensors. The limit of detection for exosomal CD44 with TIC-AFM- and TiN-NH-LSPR-biosensors was 5.

Rational Design and Effective Control of Gold-Based Bimetallic Electrocatalyst for Boosting CO Reduction Reaction: A First-Principles Study.

Electrochemical CO reduction reaction (CO RR) is an effective strategy converting CO to value-added products. Au is regarded as an efficient catalyst for electrochemical reduction of CO to CO, and the introduction of Pd can tune CO RR properties due to its strong affinity to CO. Herein, Au-Pd bimetallic electrocatalysts with different metal ratio were firstly investigated on CO RR mechanism by using density functional theory.

Preparation and photoelectrochemical properties of BiFeO/BiOI composites.

BiFeO thin films were spin coated onto FTO. BiFeO/BiOI composites have been successfully synthesized by an electrochemical deposition method. The morphology, structure and optical absorption properties of the as-synthesized samples were characterized XRD, SEM, and UV-Vis DRS.

Simultaneous Enhancement of Thermopower and Electrical Conductivity through Isovalent Substitution of Cerium in Bismuth Selenide Thermoelectric Materials.

It is challenging to achieve highly efficient thermoelectric materials due to the conflicts between thermopower (Seebeck coefficient) and electrical conductivity. These parameters are the core factors defining the thermoelectric property of any material. Here, we report the use of isovalent substitution as a tool to decouple the interdependency of the Seebeck coefficient and the electrical properties of cerium-doped bismuth selenide thermoelectric material.

Electrochemical CO Reduction to C Products on Single Nickel/Cobalt/Iron-Doped Graphitic Carbon Nitride: A DFT Study.

Electrocatalytic CO reduction reaction (CRR) is one of the most promising strategies to convert greenhouse gases to energy sources. Herein, the CRR was applied towards making C products (CO, HCOOH, CH OH, and CH ) on g-C N frameworks with single Ni, Co, and Fe introduction; this process was investigated by density functional theory. The structures of the electrocatalysts, CO adsorption configurations, and CO reduction mechanisms were systematically studied.

Label-free surface plasmon resonance biosensing with titanium nitride thin film.

In this report, titanium nitride thin film synthesized with reactive magneto-sputtering technique is proposed as an alternative surface plasmon resonance sensing material. The physical and chemical natures were initially studied by atomic force microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. In virtue of white-light common-path sensing system, the wavelength modulated TiN films achieved tunable evanescent plasmonic field from 573 nm to 627 nm.

Encapsulating Co P@C Core-Shell Nanoparticles in a Porous Carbon Sandwich as Dual-Doped Electrocatalyst for Hydrogen Evolution.

A highly efficient and pH-universal hydrogen evolution reaction (HER) electrocatalyst with a sandwich-architecture constructed using zero-dimensional N- and P-dual-doped core-shell Co P@C nanoparticles embedded into a 3 D porous carbon sandwich (Co P@N,P-C/CG) was synthesized through a facile two-step hydrothermal carbonization and pyrolysis method. The interfacial electron transfer rate and the number of active sites increased owing to the synergistic effect between the N,P-dual-doped Co P@C core-shell and sandwich-nanostructured substrates. The presence of a high surface area and large pore sizes improved the mass-transfer dynamics.

A redox-controlled electrolyte for plasmonic enhanced dye-sensitized solar cells.

Plasmonic enhanced dye-sensitized solar cells (DSSCs) with metallic nanostructures suffer from corrosion problems, especially with the presence of the iodine/triiodide redox couple in the electrolyte. Herein, we introduce an alternative approach by compensating the corrosion with a modified liquid electrolyte. In contrast to the existing method of surface preservation for plasmonic nanostructures, the redox-controlled electrolyte (RCE) contains iodoaurate intermediates, i.

Initial Reduction of CO on Pd-, Ru-, and Cu-Doped CeO(111) Surfaces: Effects of Surface Modification on Catalytic Activity and Selectivity.

Surface modification by metal doping is an effective treatment technique for improving surface properties for CO reduction. Herein, the effects of doped Pd, Ru, and Cu on the adsorption, activation, and reduction selectivity of CO on CeO(111) were investigated by periodic density functional theory. The doped metals distorted the configuration of a perfect CeO(111) by weakening the adjacent Ce-O bond strength, and Pd doping was beneficial for generating a highly active O vacancy.

Direct detection of two different tumor-derived extracellular vesicles by SAM-AuNIs LSPR biosensor.

Extracellular vesicles (EVs) are abundant in various biological fluids including blood, saliva, urine, as well as extracellular milieu. Accumulating evidence has indicated that EVs, which contain functional proteins and small RNAs, facilitate intercellular communication between neighbouring cells, and are critical to maintain various physiological processes. In contrast, EV-derived toxic signals can spread out over the tissues adjacent to the injured area in certain diseases, including brain tumors and neurodegenerative disorders.

Label-Free LSPR Detection of Trace Lead(II) Ions in Drinking Water by Synthetic Poly(mPD-co-ASA) Nanoparticles on Gold Nanoislands.

Using self-assembly gold nanoislands (SAM-AuNIs) functionalized by poly(m-phenylenediamine-co-aniline-2-sulfonic acid) (poly(mPD-co-ASA)) copolymer nanoparticles as specific receptors, a highly sensitive localized surface plasmon resonance (LSPR) optochemical sensor is demonstrated for detection of trace lead cation (Pb(II)) in drinking water. The copolymer receptor is optimized in three aspects: (1) mole ratio of mPD:ASA monomers, (2) size of copolymer nanoparticles, and (3) surface density of the copolymer. It is shown that the 95:5 (mPD:ASA mole ratio) copolymer with size less than 100 nm exhibits the best Pb(II)-sensing performance, and the 200 times diluted standard copolymer solution contributes to the most effective functionalization protocol.

Mechanical properties and failure behaviors of the interface of hybrid graphene/hexagonal boron nitride sheets.

Hybrid graphene/h-BN sheet has been fabricated recently and verified to possess unusual physical properties. During the growth process, defects such as vacancies are unavoidably present at the interface between graphene and h-BN. In the present work, typical vacancy defects, which were located at the interface between graphene and h-BN, were studied by density functional theory.

Methanol Oxidation on Pt3Sn(111) for Direct Methanol Fuel Cells: Methanol Decomposition.

PtSn alloy, which is a potential material for use in direct methanol fuel cells, can efficiently promote methanol oxidation and alleviate the CO poisoning problem. Herein, methanol decomposition on Pt3Sn(111) was systematically investigated using periodic density functional theory and microkinetic modeling. The geometries and energies of all of the involved species were analyzed, and the decomposition network was mapped out to elaborate the reaction mechanisms.

Label-free detection of 3-nitro-l-tyrosine with nickel-doped graphene localized surface plasmon resonance biosensor.

3-nitro-l-tyrosine (3-NT) is believed to be a biomarker of neurodegenerative diseases and metal doped graphene possess exceptionally high binding energy of 3-NT with metal-nitro chemisorption. Here we report a novel label-free detection scheme of 3-NT via nickel-doped graphene (NDG) as the functionalized receptor on our phase detecting localized surface plasmon resonance (LSPR) biosensor. When compared with reported 3-NT immunoassay with enzyme-linked immunosorbent assay (ELISA), our NDG-LSPR platform offers two advantages i.

Differential phase-detecting localized surface plasmon resonance sensor with self-assembly gold nano-islands.

Self-assembly (SAM) gold nano-islands are fabricated by two-step thin-film deposition-annealing method. Despite random distribution of the SAM, the p-polarized light after total internal reflection shows significant phase transition at the extinction wavelengths upon refractive index variation due to localized surface plasmon resonance (LSPR) effect. It resembles the sharp phase transition observed in conventional surface plasmon resonance (SPR) biosensors, so that the bulk sensitivity of the SAM-LSPR sensor is improved via the phase interrogation method.

Ultrathin-shell boron nitride hollow spheres as sorbent for dispersive solid-phase extraction of polychlorinated biphenyls from environmental water samples.

Boron nitride hollow spheres with ultrathin-shells were synthesized and used as sorbents for dispersive solid-phase extraction of aromatic pollutants at trace levels from environmental water samples. Polychlorinated biphenyls (PCBs) were selected as target compounds. Sample quantification and detection were performed by gas chromatography-tandem mass spectrometry.

The effect of grain boundaries on the mechanical properties and failure behavior of hexagonal boron nitride sheets.

In this work, the effect of grain boundaries (GBs) on the mechanical properties and failure behavior of two-dimensional hexagonal boron nitride (h-BN) sheets are systematically and comprehensively investigated using density functional theory. Results show that the formation of homoelemental bonds on GBs is an important factor, which could affect the atomic structures and stability of the h-BN sheet. The relationship between the formation energy and the misorientation angles is downward opening parabolic.

Common-path spectral interferometry with temporal carrier for highly sensitive surface plasmon resonance sensing.

Incorporating the temporal carrier technique with common-path spectral interferometry, we have successfully demonstrated an advanced surface plasmon resonance (SPR) biosensing system which achieves refractive index resolution (RIR) up to 2 × 10(-8) refractive index unit (RIU) over a wide dynamic range of 3 × 10(-2) RIU. While this is accomplished by optimizing the SPR differential phase sensing conditions with just a layer of gold, we managed to address the spectral phase discontinuity with a novel spectral-temporal phase measurement scheme. As the new optical setup supersedes its Michelson counterpart in term of simplicity, we believe that it is a significant contribution for practical SPR sensing applications.