Breaking the Linear Scaling Relationship of the Reverse Water–Gas–Shift Reaction via Construction of Dual-Atom Pt–Ni Pairs

Oxide-supported single-atom catalysts hold great potential for reverse water–gas–shift (RWGS) reactions. Nevertheless, it remains challenging to break the linear scaling relationships between the adsorption and desorption capability of catalysts. Herein, we report the design of ZrO2-anchored dual-atom Pt–Ni pairs for the RWGS reaction. The dual-atom material delivers a CO selectivity as high as 99.8% and a space-time yield of 157.2 μmolCO gcat–1 s–1 at atmospheric pressure. Theoretical calculations reveal that the dual-atom Pt–Ni pairs could direct the dual electronic transfer paths (dxz and dyz) to the 2π* orbitals of CO2 in the RWGS reaction, which achieve strong hybridization between them to enable efficient activation of CO2. Moreover, the delocalized charge in dual-atom Pt–Ni may lead to a facile desorption of the CO product

Breaking the Linear Scaling Relationship of the Reverse Water–Gas–Shift Reaction via Construction of Dual-Atom Pt–Ni Pairs

Oxide-supported single-atom catalysts hold great potential for reverse water–gas–shift (RWGS) reactions. Nevertheless, it remains challenging to break the linear scaling relationships between the adsorption and desorption capability of catalysts. Herein, we report the design of ZrO2-anchored dual-atom Pt–Ni pairs for the RWGS reaction. The dual-atom material delivers a CO selectivity as high as 99.8% and a space-time yield of 157.2 μmolCO gcat–1 s–1 at atmospheric pressure. Theoretical calculations reveal that the dual-atom Pt–Ni pairs could direct the dual electronic transfer paths (dxz and dyz) to the 2π* orbitals of CO2 in the RWGS reaction, which achieve strong hybridization between them to enable efficient activation of CO2. Moreover, the delocalized charge in dual-atom Pt–Ni may lead to a facile desorption of the CO product

IrCo Nanoparticles Encapsulated with Carbon Nanotubes for Efficient and Stable Acidic Water Splitting

The acidic water-splitting technology based on the polymer exchange membrane can produce hydrogen efficiently, continuously, and cleanly, which is expected to alleviate the energy crisis. However, even noble metal-based electrocatalysts such as IrOx species would dissolve rapidly during acidic oxygen evolution. Herein, we successfully assemble high-density carbon nanotubes (CNTs) encapsulated with IrCo nanoparticles (NPs) on carbon cloth (IrCo@CNT/CC) using a facile MOF-templated and dicyandiamide-assisted pyrolysis strategy. Benefiting from the favorable synergistic effect between Co and Ir and the protection of CNT, the obtained IrCo@CNT/CC only requires a low cell voltage of 1.500 V to reach 10 mA cm–2 for water splitting with an extremely low Ir loading of 0.027 mg cm–2 and exhibits robust stability under continuous electrolysis for 90 h in 0.5 M H2SO4, ranking it among one of the best bifunctional electrocatalysts for acidic water splitting. Detailed experiments reveal that the CNT-encapsulated IrCo NPs in IrCo@CNT/CC remain after the hydrogen evolution reaction (HER) but transform into Co-doped IrO2 NPs after the oxygen evolution reaction (OER). Further DFT simulation calculations confirm that the Co doping in Ir and IrO2 can optimize their electronic structures to lower their energy barriers for HER and OER, respectively

Data_Sheet_1_Exploration of the Potential Relationship Between Gut Microbiota Remodeling Under the Influence of High-Protein Diet and Crohn’s Disease.docx

Diet and gut microbiota are both important factors in the pathogenesis of Crohn’s disease, and changes in diet can lead to alteration in gut microbiome. However, there is still insufficient exploration on interaction within the gut microbiota under high-protein diet (HPD) intervention. We analyzed the gut microbial network and marker taxa from patients with Crohn’s disease in public database (GMrepo, https://gmrepo.humangut.info) combined with investigation of the changes of composition and function of intestinal microbiome in mice fed on HPD by metagenomic sequencing. The results showed that there was an indirect negative correlation between Escherichia coli and Lachnospiraceae in patients with Crohn’s disease, and Escherichia coli was a marker for both Crohn’s disease and HPD intervention. Besides, enriched HH_1414 (one of the orthologs in eggNOG) related to tryptophan metabolism was from Helicobacter, whereas reduced orthologs (OGs) mainly contributed by Lachnospiraceae after HPD intervention. Our research indicates that some compositional changes in gut microbiota after HPD intervention are consistent with those in patients with Crohn’s disease, providing insights into potential impact of altered gut microbes under HPD on Crohn’s disease.</p

IrCo Nanoparticles Encapsulated with Carbon Nanotubes for Efficient and Stable Acidic Water Splitting

The acidic water-splitting technology based on the polymer exchange membrane can produce hydrogen efficiently, continuously, and cleanly, which is expected to alleviate the energy crisis. However, even noble metal-based electrocatalysts such as IrOx species would dissolve rapidly during acidic oxygen evolution. Herein, we successfully assemble high-density carbon nanotubes (CNTs) encapsulated with IrCo nanoparticles (NPs) on carbon cloth (IrCo@CNT/CC) using a facile MOF-templated and dicyandiamide-assisted pyrolysis strategy. Benefiting from the favorable synergistic effect between Co and Ir and the protection of CNT, the obtained IrCo@CNT/CC only requires a low cell voltage of 1.500 V to reach 10 mA cm–2 for water splitting with an extremely low Ir loading of 0.027 mg cm–2 and exhibits robust stability under continuous electrolysis for 90 h in 0.5 M H2SO4, ranking it among one of the best bifunctional electrocatalysts for acidic water splitting. Detailed experiments reveal that the CNT-encapsulated IrCo NPs in IrCo@CNT/CC remain after the hydrogen evolution reaction (HER) but transform into Co-doped IrO2 NPs after the oxygen evolution reaction (OER). Further DFT simulation calculations confirm that the Co doping in Ir and IrO2 can optimize their electronic structures to lower their energy barriers for HER and OER, respectively

Interfacing with Fe–N–C Sites Boosts the Formic Acid Dehydrogenation of Palladium Nanoparticles

Hierarchical micro-/mesoporous carbons with abundant Fe–N–C sites were prepared through one-step carbonization of a metal–organic framework (MOF) with sodium iron ethylenediaminetetraacetic acid [NaFe­(III)­EDTA], which can facilitate the nucleation and growth of ultrafine (∼1.4 nm) and highly dispersed palladium nanoparticles (Pd NPs). Interfacing Pd NPs with Fe–N–C sites has been demonstrated for the first time to boost the heterogeneous catalysis of hydrogen production from formic acid, affording an ultrahigh turnover frequency (TOF) value of 7361 h–1 at 323 K. The robust synergistic interactions between Pd NPs and Fe–N–C sites together with the small size effects of Pd NPs are responsible for the enhanced catalytic activity

Silanol-Assisted High-Yield Nanofabrication of SnO₂ Single Crystals with Highly Tunable and Ordered Mesoporosity

Highly ordered mesoporous materials with a single-crystalline structure have attracted broad interest due to their wide applications from catalysis to energy conversion/storage, but constructing them with good controllability and high yields remains a highly daunting task. Herein, we construct a new class of three-dimensionally ordered mesoporous SnO2 single crystals (3DOm-SnO2) with well-defined facets and excellent mesopore tunability. Mechanism studies demonstrate that the silanol groups on ordered silica nanospheres (3DO-SiO2) can induce the efficient heterogeneous crystallization of uniform SnO2 single crystals in its periodic voids by following the hard and soft acid and base theory, affording a much higher yield of ∼96% for 3DOm-SnO2 than that of its solid counterpart prepared in the absence of 3DO-SiO2 (∼1.5%). Benefiting from its permanent ordered mesopores and favorable electronic structure, Pd-supported 3DOm-SnO2 can efficiently catalyze the unprecedented sequential hydrogenation of 4-nitrophenylacetylene to produce 4-nitrostyrene, then 4-nitroethylbenzene, and finally 4-aminoethylbenzene. DFT calculations further reveal the favorable synergistic effect between Pd and 3DOm-SnO2 via moderate electron transfer for realizing this sequential hydrogenation reaction. Our work underlines the crucial role of silanol groups in inducing the high-yield heterogeneous crystallization of 3DOm-SnO2, shedding light on the rational design and construction of various 3DO single crystals that are of great practical significance

Data_Sheet_1_Alterations in bacterial community dynamics from noncancerous to Gastric cancer.docx

Gastric microbiome has been shown to contribute to gastric carcinogenesis, understanding how alterations in gastric microbiome is helpful to the prevention and treatment of gastric cancer (GC). However, few studies have focused on the change of microbiome during the gastric carcinogenesis. In this study, the microbiome of gastric juice samples from healthy control (HC), gastric precancerous lesions (GPL) and gastric cancer (GC) was investigated by 16S rRNA gene sequencing. Our results showed that the alpha diversity of patients with GC was significantly lower than other groups. Compared to other groups, some genera in GC group were shown to be up-regulated (e.g., Lautropia and Lactobacillus) and down-regulated (e.g., Peptostreptococcus and Parvimonas). More importantly, the emergence of Lactobacillus was closely related to the occurrence and development of GC. Moreover, the microbial interactions and networks in GPL exhibited higher connectivity, complexity and lower clustering property, while GC showed the opposite trend. Taken together, we suggest that changes in the gastric microbiome are associated with GC and perform a key function in maintaining the tumor microenvironment. Therefore, our findings will provide new ideas and references for the treatment of GC.</p

Table_1_The application of metagenomic next-generation sequencing in pathogen diagnosis: a bibliometric analysis based on Web of Science.docx

BackgroundInfectious disease is a large burden on public health globally. Metagenomic next-generation sequencing (mNGS) has become popular as a new tool for pathogen diagnosis with numerous advantages compared to conventional methods. Recently, research on mNGS increases yearly. However, no bibliometric analysis has systematically presented the full spectrum of this research field. Therefore, we reviewed all the publications associated with this topic and performed this study to analyze the comprehensive status and future hotspots of mNGS for infectious disease diagnosis.MethodsThe literature was searched in the Web of Science Core Collection and screened without year or language restrictions, and the characteristics of the studies were also identified. The outcomes included publication years, study types, journals, countries, authorship, institutions, frontiers, and hotspots with trends. Statistical analysis and visualization were conducted using VOSviewer (version 1.6.16) and CiteSpace (version 6.1. R3).ResultsIn total, 325 studies were included in the analysis after screening. Studies were published between 2009 and 2022 with a significantly increasing number from 1 to 118. Most of the studies were original articles and case reports. Frontiers in Cellular and Infection Microbiology and Clinical Infectious Disease were the most commonly cited and co-cited journals. Institutions and researchers from China contributed the most to this field, followed by those from the USA. The hotspots and frontiers of these studies are pneumonia, tuberculosis, and central nervous system infections.ConclusionThis study determined that mNGS is a hot topic in the diagnosis of infectious diseases with development trends and provides insights into researchers, institutions, hotspots and frontiers in mNGS, which can offer references to related researchers and future research.</p

Controlled Growth of Monodisperse Ferrite Octahedral Nanocrystals for Biomass-Derived Catalytic Applications

Metal/metal oxide nanoparticles with controllable size and shape are of importance to tailor the catalytic performances of metal nanoparticles. However, a facile synthesis of supported monodisperse metal/oxide polyhedra in the absence of capping agents remains a significant challenge, especially at high metal loadings. In this work, a surfactant-free MOF (metal–organic framework) thermolysis strategy is developed for the synthesis of monodisperse ferrite octahedral nanocrystals with uniform composition for the first time. The achievement of our synthesis relies on the use of CO as directing agent that may control the growth rate of specific facets at the solid/gas interface and, subsequently, the shape of the resultant metal oxide nanostructures. As-prepared octahedral ferrite materials exhibited an interesting shape-dependent catalytic performance in 5-hydroxymethylfurfural (HMF) oxidation, achieving significantly improved activity and selectivity, compared to those synthesized under a pure inert atmosphere. Density functional theory (DFT) calculations suggest a relatively weak interaction between 2,5-diformylfuran (DFF) and the catalyst that is highly beneficial for product desorption, avoiding the overoxidation reactions that occur on the catalyst surface to some extent and partially contributing to the high DFF selectivity