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Background: Multiple studies have shown that tumor-associated macrophages (TAMs) promote cancer initiation and progression. However, the reprogramming of macrophages in the tumor microenvironment (TME) and the cross-talk between TAMs and malignant subclones in intrahepatic cholangiocarcinoma (iCCA) has not been fully characterized, especially in a spatially resolved manner. Deciphering the spatial architecture of variable tissue cellular components in iCCA could contribute to the positional context of gene expression containing information pathological changes and cellular variability. Methods: Here, we applied spatial transcriptomics (ST) and digital spatial profiler (DSP) technologies with tumor sections from patients with iCCA. Results: The results reveal that spatial inter- and intra-tumor heterogeneities feature iCCA malignancy, and tumor subclones are mainly driven by physical proximity. Tumor cells with TME components shaped the intra-sectional heterogenetic spatial architecture. Macrophages are the most infiltrated TME component in iCCA. The protein trefoil factor 3 (TFF3) secreted by the malignant subclone can induce macrophages to reprogram to a tumor-promoting state, which in turn contributes to an immune-suppressive environment and boosts tumor progression. Conclusions: In conclusion, our description of the iCCA ecosystem in a spatially resolved manner provides novel insights into the spatial features and the immune suppressive landscapes of TME for iCCA. [ABSTRACT FROM AUTHOR]

Since the facile oxidation of ammonia is one key for its utilization as a zero‐carbon fuel in a direct ammonia fuel cell, developing the ammonia oxidation reaction (AOR) catalysts with cost‐effective and higher activity is urgently required. However, the catalytic activity of AOR is limited by the scaling relationship of the intermediate adsorption. Based on the density functional theory, the N‐modified Co3Mo3C with separated active sites of NH3 dehydrogenation and N−N coupling has been designed and investigated, which is a promising strategy to circumvent the scaling relationship, achieving improved AOR catalytic performance with a lower theoretical overpotential of 0.59 V under fast reaction kinetics condition. The calculation results show that the hollow site (Co−Mo−Mo and Co−Co−Mo) and Co site in N‐modified Co3Mo3C play essential roles in NH3 dehydrogenation and N−N coupling, respectively. This work not only benefits for understanding the mechanism of AOR, but also provides a fundamental guidance for rational design of AOR catalysts. [ABSTRACT FROM AUTHOR]

With the advantage of fast charge transfer, heterojunction engineering is identified as a viable method to reinforce the anodes' sodium storage performance. Also, vacancies can effectively strengthen the Na+ adsorption ability and provide extra active sites for Na+ adsorption. However, their synchronous engineering is rarely reported. Herein, a hybrid of Co0.85Se/WSe2 heterostructure with Se vacancies and N‐doped carbon polyhedron (CoWSe/NCP) has been fabricated for the first time via a hydrothermal and subsequent selenization strategy. Spherical aberration‐corrected transmission electron microscopy confirms the phase interface of the Co0.85Se/WSe2 heterostructure and the existence of Se vacancies. Density functional theory simulations reveal the accelerated charge transfer and enhanced Na+ adsorption ability, which are contributed by the Co0.85Se/WSe2 heterostructure and Se vacancies, respectively. As expected, the CoWSe/NCP anode in sodium‐ion battery achieves outstanding rate capability (339.6 mAh g−1 at 20 A g−1), outperforming almost all Co/W‐based selenides. [ABSTRACT FROM AUTHOR]

Sodium-ion batteries have emerged as competitive substitutes for low-temperature applications due to severe capacity loss and safety concerns of lithium-ion batteries at - 20 °C or lower. However, the key capability of ultrafast charging at ultralow temperature for SIBs is rarely reported. Herein, a hybrid of Bi nanoparticles embedded in carbon nanorods is demonstrated as an ideal material to address this issue, which is synthesized via a high temperature shock method. Such a hybrid shows an unprecedented rate performance (237.9 mAh g -1 at 2 A g -1 ) at - 60 °C, outperforming all reported SIB anode materials. Coupled with a Na 3 V 2 (PO 4 ) 3 cathode, the energy density of the full cell can reach to 181.9 Wh kg -1 at - 40 °C. Based on this work, a novel strategy of high-rate activation is proposed to enhance performances of Bi-based materials in cryogenic conditions by creating new active sites for interfacial reaction under large current., Competing Interests: Declarations Conflict of interest The authors declare no interest conflict. They have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (© 2024. The Author(s).)

Developing economical and efficient electrocatalysts is critical for hydrogen energy industrialization through water electrolysis. Herein, a novel dual-site synergistic NiFe/Y 2 O 3 hybrid with abundant interfacial Ni/Fe─O─Y bonds is designed by density functional theory (DFT) simulations. In situ Raman spectra combined with DFT calculations reveal that the interfacial Ni/Fe─O─Y units greatly promote H 2 O dissociation and optimize the adsorption of both H* and oxygen species, achieving excellent activity and durability for hydrogen evolution reaction. As expected, NiFe/Y 2 O 3 exhibits a low overpotential of 27 mV at 10 mA cm -2 and robust stability of over 200 h at 1000 mA cm -2 , and also outstanding water splitting performance with a low cell voltage of 1.64 V at 100 mA cm -2 , showing significant potential for real-world applications., (© 2024 Wiley‐VCH GmbH.)

With the advantages of a Fenton-inactive characteristic and unique p electrons that can hybridize with O 2 molecules, p-block metal-based single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) have tremendous potential. Nevertheless, their undesirable intrinsic activity caused by the closed d 10 electronic configuration remains a major challenge. Herein, an Sb-based SAC featuring carbon vacancy-enhanced Sb-N 4 active centers, corroborated by the results of high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure, has been developed for an incredibly effective ORR. The obtained Sb SA -N-C demonstrates a positive half-wave potential of 0.905 V and excellent structural stability in alkaline environments. Density functional theory calculations reveal that the carbon vacancies weaken the adsorption between Sb atoms and the OH* intermediate, thus promoting the ORR performance. Practically, the Sb SA -N-C-based Zn-air batteries achieve impressive outcomes, such as a high power density of 181 mW cm -2 , showing great potential in real-world applications.

Since the facile oxidation of ammonia is one key for its utilization as a zero-carbon fuel in a direct ammonia fuel cell, developing the ammonia oxidation reaction (AOR) catalysts with cost-effective and higher activity is urgently required. However, the catalytic activity of AOR is limited by the scaling relationship of the intermediate adsorption. Based on the density functional theory, the N-modified Co 3 Mo 3 C with separated active sites of NH 3 dehydrogenation and N-N coupling has been designed and investigated, which is a promising strategy to circumvent the scaling relationship, achieving improved AOR catalytic performance with a lower theoretical overpotential of 0.59 V under fast reaction kinetics condition. The calculation results show that the hollow site (Co-Mo-Mo and Co-Co-Mo) and Co site in N-modified Co 3 Mo 3 C play essential roles in NH 3 dehydrogenation and N-N coupling, respectively. This work not only benefits for understanding the mechanism of AOR, but also provides a fundamental guidance for rational design of AOR catalysts., (© 2023 Wiley‐VCH GmbH.)