Highly exposed metal atomic active sites in Al2O3/CoNC: Modify reaction pathways by coupling oxygen species.

The catalytic oxidation of formaldehyde (HCHO) at ambient temperature is a highly efficient, cost-effective and environmentally friendly approach for formaldehyde removal. Reactive oxygen (O*) and reactive hydroxyl groups (OH*) are the main active species in the catalytic oxidation reaction of HCHO. Therefore, it is crucial to design catalysts that can simultaneously enhance the surface concentrations of O* and OH*, thereby improving their overall catalytic performance. The present study aimed to design an Al2O3/CoNC catalyst featuring layered carbon nitride coupled with metal oxides possessing domain-limited cobalt (Co) metal active sites, to efficiently remove HCHO (≈100 %, 100 ppm, RH=50 %, GSHV=20,000 mL/(g h)) and ensure stability (more than 90 % formaldehyde removal within 450 h) at ambient temperature. The characterization revealed that the interaction between Al2O3-supported metal and CoNC resulted in enhanced confinement of Co, leading to a higher abundance of edge structures exposing more active sites. Additionally, the presence of highly dispersed Co-NX active sites and increased oxygen vacancies effectively facilitated the adsorption and activation processes of HCHO and O2, as well as the adsorption and desorption dynamics of intermediates during the reaction. These factors collectively contributed to an improved catalytic activity. The results of in situ infrared spectroscopy revealed that the catalyst improved the adsorption and activation of O2 and H2O, leading to the rapid generation of substantial amounts of O* and OH*. This synergistic interaction between Al2O3 and CoNC plays a crucial role in the sustained production of O* and OH*, promoting efficient of intermediate decomposition, and ensuring excellent catalytic activity and stability for HCHO.

Structurally disordered MoSe2 with rich 1T phase as a universal platform for enhanced photocatalytic hydrogen production.

The improvement of surface reactivity in noble-metal-free cocatalysts is crucial for the development of efficient and cost-effective photocatalytic systems. However, the influence of crystallinity on catalytic efficacy has received limited attention. Herein, we report the utilization of structurally disordered MoSe2 with abundant 1T phase as a versatile cocatalyst for photocatalytic hydrogen evolution. Using MoSe2/carbon nitride (CN) hybrids as a case study, it is demonstrated that amorphous MoSe2 significantly enhances the hydrogen evolution rate of CN, achieving up to 11.37 µmol h-1, surpassing both low crystallinity (8.24 µmol h-1) and high crystallinity MoSe2 (3.86 µmol h-1). Experimental analysis indicates that the disordered structure of amorphous MoSe2, characterized by coordination-unsaturated surface sites and a rich 1T phase with abundant active sites at the basal plane, predominantly facilitates the conversion of surface-bound protons to hydrogen. Conversely, the heightened charge transfer capacity of the highly crystalline counterpart plays a minor role in enhancing practical catalytic performance. This approach is applicable for enhancing the photocatalytic hydrogen evolution performance of various semiconducting photocatalysts, including CdS, TiO2, and ZnIn2S4, thereby offering novel insights into the advancement of high-performance non-precious catalysts through phase engineering.

One-dimensional Ga2O3-Al2O3 nanofibers with unsaturated coordination Ga: Catalytic dehydrogenation of propane under CO2 atmosphere with excellent stability.

The pressing demand for propylene has spurred intensive research on the catalytic dehydrogenation of propane to produce propylene. Gallium-based catalysts are regarded as highly promising due to their exceptional dehydrogenation activity in the presence of CO2. However, the inherent coking issue associated with high temperature reactions poses a constraint on the stability development of this process. In this study, we employed the electrospinning method to prepare a range of Ga2O3-Al2O3 mixed oxide one-dimensional nanofiber catalysts with varying molar ratios for CO2 oxidative dehydrogenation of propane (CO2-OPDH). The propane conversion was up to 48.4 % and the propylene selectivity was high as 96.8 % at 500 °C, the ratio of propane to carbon dioxide is 1:2. After 100 h of reaction, the catalyst still maintains approximately 10 % conversion and exhibits a propylene selectivity of around 98 %. The electrospinning method produces one-dimensional nanostructures with a larger specific surface area, unique multi-stage pore structure and low-coordinated Ga3+, which enhances mass transfer and accelerates reaction intermediates. This results in less coking and improved catalyst stability. The high activity of the catalyst is attributed to an abundance of low-coordinated Ga3+ ions associated with weak/medium-strong Lewis acid centers. In situ infrared analysis reveals that the reaction mechanism involves a two-step dehydrogenation via propane isocleavage, with the second dehydrogenation of Ga-OR at the metal-oxygen bond being the decisive speed step.

Climate match is key to predict range expansion of the world's worst invasive terrestrial vertebrates.

Understanding the determinants of the range expansion of invasive alien species is crucial for developing effective prevention and control strategies. Nevertheless, we still lack a global picture of the potential factors influencing the invaded range expansion across taxonomic groups, especially for the world's worst invaders with high ecological and economic impacts. Here, by extensively collecting data on 363 distributional ranges of 19 of world's worst invasive terrestrial vertebrates across 135 invaded administrative jurisdictions, we observed remarkable variations in the range expansion across species and taxonomic groups. After controlling for taxonomic and geographic pseudoreplicates, model averaging analyses based on generalized additive mixed-effect models showed that species in invaded regions having climates more similar to those of their native ranges tended to undergo a larger range expansion. In addition, as proxies of propagule pressure and human-assisted transportation, the number of introduction events and the road network density were also important predictors facilitating the range expansion. Further variance partitioning analyses validated the predominant role of climate match in explaining the range expansion. Our study demonstrated that regions with similar climates to their native ranges could still be prioritized to prevent the spread of invasive species under the sustained global change.

Novel synergistically effects of palladium-iron bimetal and manganese carbonate carrier for catalytic oxidation of formaldehyde at room temperature.

The elimination of formaldehyde at room temperature holds immense potential for various applications, and the incorporation of a catalyst rich in surface hydroxyl groups and oxygen significantly enhances its catalytic activity towards formaldehyde oxidation. By employing a coprecipitation method, we successfully achieved a palladium domain confined within the manganese carbonate lattice and doped with iron. This synergistic effect between highly dispersed palladium and iron greatly amplifies the concentration of surface hydroxyl groups and oxygen on the catalyst, thereby enabling complete oxidation of formaldehyde at ambient conditions. The proposed method facilitates the formation of domain-limited palladium within the MnCO3 lattice, thereby enhancing the dispersion of palladium and facilitating its partial incorporation into the MnCO3 lattice. Consequently, this approach promotes increased exposure of active sites and enhances the catalyst's capacity for oxygen activation. The co-doping of iron effectively splits the doping sites of palladium to further enhance its dispersion, while simultaneously modifying the electronic modification of the catalyst to alter formaldehyde's adsorption strength on it. Manganese carbonate exhibits superior adsorption capability for activated surface hydroxyl groups due to the presence of carbonate. In situ infrared testing revealed that dioxymethylene and formate are primary products resulting from catalytic oxidation of formaldehyde, with catalyst surface oxygen and hydroxyl groups playing a crucial role in intermediate product decomposition and oxidation. This study provides novel insights for designing palladium-based catalysts.

TARF: Technology-Agnostic RF Sensing for Human Activity Recognition.

With the rapid development towards smart Internet of Things (IoT), detection of human activity has become essential in a variety of applications. Various radio-frequency (RF) sensing technologies, such as WiFi, Radio-Frequency Identification (RFID), and Frequency-Modulated Continuous Wave (FMCW) radar, have been utilized for non-invasive human activity recognition (HAR). It will be highly desirable to develop a HAR solution that can work with different types of RF technologies, such that the cost and the barrier of wide deployment can both be greatly reduced, and more robust performance can be achieved by utilizing the complementary RF sensory data. In this paper, we propose a technology-agnostic approach for RF-based HAR, termed TARF, which works with several different RF sensing technologies. A novel data generalization technique is proposed to mitigate the disparity in measured data from different RF devices. A domain adversarial neural network is proposed to combat the interference from various RF sensing technologies. The performance of the proposed system is evaluated with experiments using four different RF sensing technologies. TARF is shown to outperform the state-of-the-art Convolutional Neural Network (CNN)-based solution with considerable gains.

Biological invasions facilitate zoonotic disease emergences.

Outbreaks of zoonotic diseases are accelerating at an unprecedented rate in the current era of globalization, with substantial impacts on the global economy, public health, and sustainability. Alien species invasions have been hypothesized to be important to zoonotic diseases by introducing both existing and novel pathogens to invaded ranges. However, few studies have evaluated the generality of alien species facilitating zoonoses across multiple host and parasite taxa worldwide. Here, we simultaneously quantify the role of 795 established alien hosts on the 10,473 zoonosis events across the globe since the 14th century. We observe an average of ~5.9 zoonoses per alien zoonotic host. After accounting for species-, disease-, and geographic-level sampling biases, spatial autocorrelation, and the lack of independence of zoonosis events, we find that the number of zoonosis events increase with the richness of alien zoonotic hosts, both across space and through time. We also detect positive associations between the number of zoonosis events per unit space and climate change, land-use change, biodiversity loss, human population density, and PubMed citations. These findings suggest that alien host introductions have likely contributed to zoonosis emergences throughout recent history and that minimizing future zoonotic host species introductions could have global health benefits.

Enabling Efficient Aerobic 5-Hydroxymethylfurfural Oxidation to 2,5-Furandicarboxylic Acid in Water by Interfacial Engineering Reinforced Cu-Mn Oxides Hollow Nanofiber.

Herein, a one-dimensional hollow nanofiber catalyst composed of tightly packed multiphase metal oxides of Mn2 O3 and Cu1.4 Mn1.6 O4 was constructed by electrospinning and tailored thermal treatment procedure. The characterization results comprehensively confirmed the special morphology and composition of various comparative catalysts. This strategy endowed the catalyst with abundant interfacial characteristics of components Mn2 O3 and Cu1.4 Mn1.6 O4 nanocrystal. Impressively, the tuning thermal treatment resulted in tailored CuI sites and surface oxygen species of the catalyst, thus affording optimized oxygen vacancies for reinforced oxygen adsorption, while the concomitant enhanced lattice oxygen activity in the constructed composite catalyst ensured the higher catalytic oxidation ability. More importantly, the regulated proportion of oxygen vacancy and lattice oxygen in the composite catalyst was obtained in the best catalyst, beneficial to accelerate the reaction cycle. Compared to other counterparts obtained by different temperatures, the CMO-500 sample exhibited superior selective aerobic 5-hydroxymethylfurfural (HMF) oxidation to 2,5-furandicarboxylic acid (FDCA, 96 % yield) in alkali-bearing aqueous solution using O2 at 120 °C, which resulted from the above-mentioned composition optimization and interfacial engineering reinforced surface oxygen consumption and regeneration cycle. The reaction mechanism was further proposed to uncover the lattice oxygen and oxygen vacancy participating HMF conversion process.

Interfacial engineering coupling with tailored oxygen vacancies in Co2Mn2O4 spinel hollow nanofiber for catalytic phenol removal.

Herein, one-dimensional Co2Mn2O4 (CMO) hollow nanofibers with a general spinel structure were constructed by electrospinning and tunning thermal-driven procedures. The resultant catalyst was endowed with appreciable active interfacial engineering effect, which revealed improved peroxymonosulfate (PMS) activation efficiency in catalytic phenol degradation with nearly 12.9 folds increment in reaction rate constant compared to the hydrothermally synthesized counterpart. Besides, tailored oxygen-vacancy sites including chemical environment and contents in the bimetallic spinel were rationally validated compared to the monometal spinel counterparts. The improved catalytic phenol degradation by reactive-oxidative-species (ROS) from PMS was well correlated with the more active Co(II) and Mn(II) species, reactive active oxygen-vacancy and the interfacial engineering effect in the CMO catalyst. These correlations were comprehensively demonstrated by various characterization techniques, catalytic results, and Density-Functional-Theoretical (DFT) calculations of the adsorption and activation of PMS. Besides, the results revealed that the specific content of cobalt species in the structural unit of the Co2Mn2O4 spinel resulting from the optimized thermal treatment could further improve the catalytic activity by the intermetallic synergy along with the beneficial electron transfer cycles. This work provides a practical understanding of the improvement of interfacial systems in catalysis efficiency and environmental remediation.

Reductive C-N Coupling of Nitroarenes: Heterogenization of MoO3 Catalyst by Confinement in Silica.

The construction of C-N bonds with nitroaromatics and boronic acids using highly efficient and recyclable catalysts remains a challenge. In this study, nanoporous MoO3 confined in silica serves as an efficient heterogeneous catalyst for C-N cross-coupling of nitroaromatics with aryl or alkyl boronic acids to deliver N-arylamines and with desirable multiple reusability. Experimental results suggest that silica not only heterogenizes the Mo species in the confined mesoporous microenvironment but also significantly reduces the reaction induction period and regulates the chemical efficiency of the targeted product. The well-shaped MoO3 @m-SiO2 catalyst exhibits improved catalytic performance both in yield and turnover number, in contrast with homogeneous Mo catalysts, commercial Pd/C, or MoO3 nanoparticles. This approach offers a new avenue for the heterogeneous catalytic synthesis of valuable bioactive molecules.

Visible-Light-Responsive Nanofibrous α-Fe2O3 Integrated FeOx Cluster-Templated Siliceous Microsheets for Rapid Catalytic Phenol Removal and Enhanced Antibacterial Activity.

Visible-light-driven environmental contaminants control using 2D photocatalytic nanomaterials with an unconfined reaction-diffusion path is advantageous for public health. Here, cost-effective siliceous composite microsheets (FeSiO-MS) combined with two distinct refined α-Fe2O3 nanospecies as photofunctional catalysts were constructed via a one-pot synthesis approach. Through precise control of Fe2+ precursor addition, specially configured α-Fe2O3 nanofibers combined with FeOx cluster-functionalized siliceous microsheets of ∼15 nm gradually evolved from the iron oxide-bearing molecular sieve, endowing a superior light-response characteristic of the formed nanocomposite. The catalytic experiment along with the ESR study demonstrated that the produced FeSiO-MS showed reinforced photo-Fenton reactivity, which was effective for rapid phenol degradation under visible light radiation. Moreover, the phenol removal process was found to be regulated by the specially configured types and concentrations of iron oxides. Notably, the obtained composites exhibited a considerable visible-light-induced bactericidal effect against E. coli. The constructed FeSiO-MS nanocomposites as integrated and eco-friendly photocatalysts exhibit enormous potentials for environmental and hygienic application.

Loading of individual Se-doped Fe2O3-decorated Ni/NiO particles on carbon cloth: facile synthesis and efficient electrocatalysis for the oxygen evolution reaction.

The synthesis of competitive, affordable and sustainable electrocatalysts via simple and scalable methods is highly desirable for the oxygen evolution reaction (OER). Usually, expensive, complex, time-consuming methods are applied to prepared suitable electrocatalysts for the OER. In contrast, a single-step thermal method is simple and inexpensive. Nickel and iron-based composite materials are potential candidates as OER catalysts. Accordingly, herein, Se-doped Fe2O3-decorated Ni/NiO particles on carbon cloth (Se-Fe2O3@Ni/NiO/CC) were synthesized via a facile and scalable one-step thermal method. The individual Se-Fe2O3@Ni/NiO particles were accommodated in holes in the carbon fibers of CC. The optimized Se-Fe2O3@Ni/NiO/CC-2 sample exhibited an outstanding OER performance with an overpotential of 205 mV at the current density 10 mA cm-2, small Tafel slope of 36 mV dec-1, and good stability in 1.0 M KOH electrolyte. The outstanding catalytic performance was mainly attributed to the heterointerfaces between Se-Fe2O3 and Se-Ni/NiO. Moreover, the accommodation of the Se-Fe2O3@Ni/NiO particles in the holes of CC restricted the aggregation of the particles, and CC provided a conductive substrate for the OER process. Thus, this work provides a simple, scalable and effective strategy for designing and engineering of outstanding electrocatalysts for the OER.

Animal invaders threaten protected areas worldwide.

Protected areas are the cornerstone of biodiversity conservation. However, alien species invasion is an increasing threat to biodiversity, and the extent to which protected areas worldwide are resistant to incursions of alien species remains poorly understood. Here, we investigate establishment by 894 terrestrial alien animals from 11 taxonomic groups including vertebrates and invertebrates across 199,957 protected areas at the global scale. We find that <10% of protected areas are home to any of the alien animals, but there is at least one established population within 10-100 km of the boundaries of 89%-99% of protected areas, while >95% of protected areas are environmentally suitable for establishment. Higher alien richness is observed in IUCN category-II national parks supposedly with stricter protection, and in larger protected areas with higher human footprint and more recent designation. Our results demonstrate that protected areas provide important protection from biological invasions, but invasions may become an increasingly dominant problem in the near future.

Surface defective g-C3N4-xClx with unique spongy structure by polarization effect for enhanced photocatalytic removal of organic pollutants.

Natural sponge is an ancient marine organism with a single lamellar structure, on which there are abundant porous channels to compose full-fledged spatial veins. Illumined by the natural spongy system, herein, the Cl doped surface defective graphite carbon nitride (g-C3N4-xClx) was constructed through microwave etching. In this process, microwave with HCl was employed to produce surface defects and peel bulk g-C3N4 to form natural spongy structured g-C3N4-xClx with three-dimensional networks. The spongy structure of the photocatalyst could provide abundant and unobstructed pathways for the transfer and separation of electron-hole pairs, and it was beneficial for photocatalytic reaction. The spongy defective g-C3N4-xClx achieved excellent degradation of diclofenac sodium (100%), bisphenol A (88.2%), phenol (85.7%) and methylene blue (97%) solution under simulated solar irradiation, respectively. The chlorine atoms were introduced into the g-C3N4 skeleton in microwave field with HCl, forming C-Cl bonds and surface polarization field, which could significantly accelerate the separation of photogenerated electrons and holes. As an efficient and universal approach, microwave etching can be generally used to create surface defects for most photocatalysts, which may have potential applications in environmental purification, energy conversion and photodynamic therapy.

Strategy for stabilizing noble metal nanoparticles without sacrificing active sites.

We report a facile surface fluorination strategy for restricting Pt nanoparticle sintering through providing anchoring sites on the TiO2 support and enhancing metal-support interaction via improved electronic interaction without sacrificing the active sites. The fluorine-tailored Pt/TiO2 exhibits excellent sintering resistance and significant activity enhancement in the catalytic oxidation of toluene.