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Square platform Cu2MoS4/lamellar ZnIn2S4 composites were prepared for enhancing the photocatalytic activity. The loading of lamellar ZnIn2S4 on the surface of Cu2MoS4 can improve the photocatalytic hydrogen evolution efficiency.

This review focuses on the application of g-C3N4 combined with ZIF series, MIL series, UIO series and other MOF materials in photocatalytic hydrogen production and carbon dioxide reduction, and summarizes the resulting photocatalytic performance of the various composites.

Arteriosclerosis Obliteran (ASO) is a local manifestation of systemic arteriosclerosis in the lower extremity arteries. ASO is a chronic progressive disease caused by arteriosclerosis, such as intimal thickening, lumen stenosis or occlusion of the blood supply arteries of the lower limbs, insufficient blood supply of the diseased limbs, and clinical manifestations such as intermittent claudication, decreased skin temperature, pain, and even ulceration or necrosis of the lower limbs. Its pathogenesis is complex, the treatment is difficult and has gradually attracted extensive attention in clinic. In recent years, more and more studies have shown that hyperhomocysteinemia is an independent risk factor of atherosclerosis, but there is no clinical report on hyperhomocysteinemia and ASO. Therefore, this paper reviews the correlation between hyperhomocysteinemia and ASO, in order to provide theoretical basis and support for the follow-up study of ASO.

The physics reach of the LHCb detector can be extended by reconstructing particles with a long lifetime that decay downstream of the dipole magnet, using only hits in the furthest tracker from the interaction point. This allows for electromagnetic dipole moment measurements, and increases the reach of beyond the Standard Model long-lived particle searches. However, using tracks to reconstruct particles decaying in this region is challenging, particularly due to the increased combinatorics and reduced momentum and vertex resolutions, which is why it has not been done until now. New approaches have been developed to meet the challenges and obtain worthwhile physics from these previously unused tracks. This talk presents the feasibility demonstration studies performed using Run-2 data, as well as new developments that expand these techniques for further gains in Run-3.

[Image: see text] Based on the pathological mechanisms of acute kidney injury (AKI), a stepwise targeting curcumin derivative, Ser@TPP@CUR, was developed in this study. Ser@TPP@CUR can be specifically internalized by renal tubular epithelial cells via KIM-1 receptor-mediated endocytosis and then actively distributed in mitochondria under the effect of TPP, a mitochondrial targeting molecule. Both in vitro and in vivo results showed that Ser@TPP@CUR effectively ameliorated injured renal tubular epithelial cells and improved renal functions of AKI mice.

Conversion into high-value-added organic nitrogen compounds through electrochemical C-N coupling reactions under ambient conditions is regarded as a sustainable development strategy to achieve carbon neutrality and high-value utilization of harmful substances. Herein, we report an electrochemical process for selective synthesis of high-valued formamide from carbon monoxide and nitrite with a Ru1Cu single-atom alloy under ambient conditions, which achieves a high formamide selectivity with Faradaic efficiency of 45.65 ± 0.76% at −0.5 V vs. RHE. In situ X-ray absorption spectroscopy, coupled with in situ Raman spectroscopy and density functional theory calculations results reveal that the adjacent Ru-Cu dual active sites can spontaneously couple *CO and *NH2 intermediates to realize a critical C-N coupling reaction, enabling high-performance electrosynthesis of formamide. This work offers insight into the high-value formamide electrocatalysis through coupling CO and NO2− under ambient conditions, paving the way for the synthesis of more-sustainable and high-value chemical products.

High-entropy-alloy (HEA) nanocrystals consisting of a minimum of five elements have recently emerged as a versatile family of catalysts due to immense chemical space and tunability1-3. However, there are no effective strategies for synthesizing libraries of HEA nanocrystals with controlled surface atomic structures of exposed facets for boosting catalytic performance4-19. Due to the distinct nucleation and growth kinetics of constituent metals and their distinctive crystal structures, it is incredibly challenging to confine five or more different metal species situated on the nanocrystal surface with a specific arrangement but also in a high-entropy random mixing state. Here we present a straightforward strategy to craft a library of facet-controlled HEA nanocrystals with up to ten dissimilar metallic elements (Pt, Pd, Ir, Ru, Rh, Os, Au, Fe, Co, and Ni) by solution-phase layer-by-layer epitaxial growth, enabling the design of 638 distinct catalysts with 5 to 10 elements in equimolar ratios. The subnanometer-thick solid-solution HEA atomic layers can be deposited epitaxially on nanocrystal seeds with {100} and {111} facets, thus achieving HEA shells with square and hexagonal atomic arrangements, respectively. The hollow HEA nanocages with ultrathin walls along a specific direction can be further fabricated via post-synthetic chemical etching. Three facet-dependent catalytic actives of HEA nanocrystals are discovered in electrocatalysis and photocatalysis, and their catalytic facets with real active sites are also identified by in situ synchrotron X-ray absorption spectroscopy and density-functional theory calculations. Our work enables facet engineering in the multi-elemental space and unveils the critical needs for their future development toward catalysis.

A novel catalyst consisting of Ir single atoms confined in porous N, S co-doped Ti3C2Tx is successfully constructed through a gelation-and-pyrolysis method, which shows remarkable catalytic activity towards the HER in acidic and basic electrolytes.

Providing affordable safe drinking water and universal sanitation poses a grand challenge especially after the global COVID-19 pandemic. In this work, we developed atomically dispersed Au on potassium-incorporated polymeric carbon nitride (AuKPCN) that could simultaneously boost photocatalytic generation of ·OH and H2O2 with an apparent quantum efficiency over 90% at 400–420 nm. The introduction of potassium into the poly(heptazine imide) matrix formed strong K-N bonds, preventing Au from forming strong interactions with N. Instead, Au formed a bond with C, only having weak interactions with N on KPCN, which rendered Au with an oxidation number close to 0. The results of in-situ vibrational spectroscopy, isotopic experiments, transient absorption spectroscopy and time-dependent density functional theory (TDDFT) simulations revealed that the low-valent Au could append its 6s orbital into the band diagram of AuKPCN that formed a trapping level for generating highly localized holes under photoexcitation. These highly localized holes could boost the 1e− water oxidation reaction to form highly oxidative ·OH and simultaneously unbind the hydrogen atom in H2O molecule, which greatly promoted the hydrogenation process during the 2e− oxygen reduction reaction (ORR) to produce H2O2. The photogenerated ·OH on AuKPCN led to a more than 120-fold efficiency enhancement for visible-light-response superhydrophilicity as compared to that of the commercial TiO2. The onsite fixed-bed reactor under photo-illumination achieved a remarkable 132.5 LH2O m− 2 day− 1 water disinfection rate (lg6), which is about 30 times superior than the TiO2 photocatalytic advanced oxidation process in the most ideal case (H2O m− 2 day− 1; lg4).

Single-atom catalysts with a well-defined metal center open unique opportunities for exploring the catalytically active site and reaction mechanism of chemical reactions. However, understanding of the electronic and structural dynamics of single-atom catalytic centers under reaction condition is still limited due to the challenge of combining operando techniques that are sensitive to such sites and model single-atom systems. Herein, supported by state-of-the-art operando techniques, we provide an in-depth study of the dynamic structural and electronic evolution during electrochemical CO2 reduction reaction (CO2RR) of a model catalyst comprising iron only as a high-spin (HS) Fe(III)N4 center in its resting state. Operando 57Fe Mössbauer and X-ray absorption spectroscopies clearly evidence the change from a HS Fe(III)N4 to a HS Fe(II)N4 center with decreasing potential, CO2- or Ar-saturation of the electrolyte leading to different adsorbates and stability of the HS Fe(II)N4 center. With operando Raman spectroscopy and cyclic voltammetry, we identify that the phthalocyanine (Pc) ligand coordinating the iron cation center undergoes a redox process from Fe(II)Pc to Fe(II)Pc−. Altogether, the HS Fe(II)Pc− species is identified as the catalytic intermediate for CO2RR. Furthermore, theoretical calculations reveal that the electroreduction of the Pc ligand modifies the d-band center of the in situ generated HS Fe(II)Pc− species, resulting in an optimal binding strength to CO2 and thus boosting the catalytic performance of CO2RR. This work provides both experimental and theoretical evidence towards the electronic structural and dynamics of reactive sites in single-Fe-atom materials and shall guide the design of novel efficient catalysts for CO2RR.

A nanoporous Pd50Ir50 alloy is developed for water splitting bifunctional electrocatalysis by metallurgical alloy design and electrochemical dealloying method, outperforming the state-of-the-art catalysts, commercial Pt/C and Ir/C under 0.5 M H2SO4.

Resource limitations make it hard to provide all students with one of the most effective educational interventions: personalized instruction. Reinforcement learning could be a key tool to reduce the development cost and improve the effectiveness of intelligent tutoring software that aims to provide the right support, at the right time, to a student. Here we illustrate that deep reinforcement learning can be used to provide adaptive pedagogical support to students learning about the concept of volume in a narrative storyline software. Using explainable artificial intelligence tools, we extracted interpretable insights about the pedagogical policy learned and demonstrated that the resulting policy had similar performance in a different student population. Most importantly, in both studies, the reinforcement-learning narrative system had the largest benefit for those students with the lowest initial pretest scores, suggesting the opportunity for AI to adapt and provide support for those most in need., Comment: 23 pages. Under review

Heteroatom doped atomically dispersed Fe1 -NC catalysts have been found to show excellent activity toward oxygen reduction reaction (ORR). However, the origin of the enhanced activity is still controversial because the structure-function relationship governing the enhancement remains elusive. Herein, sulfur(S)-doped Fe1 -NC catalyst was obtained as a model, which displays a superior activity for ORR towards the traditional Fe-NC materials. 57 Fe Mossbauer spectroscopy and electron paramagnetic resonance spectroscopy revealed that incorporation of S in the second coordination sphere of Fe1 -NC can induce the transition of spin polarization configuration. Operando 57 Fe Mossbauer spectra definitively identified the low spin single-Fe3+ -atom of C-FeN4 -S moiety as the active site for ORR. Moreover, DFT calculations unveiled that lower spin state of the Fe center after the S doping promotes OH* desorption process. This work elucidates the underlying mechanisms towards S doping for enhancing ORR activity, and paves a way to investigate the function of broader heteroatom doped Fe1 -NC catalysts to offer a general guideline for spin-state-determined ORR.

Single-atom catalysts have attracted extensive attention due to their unique atomic structures and extraordinary activities in catalyzing chemical reactions. However, the lack of general and efficient approaches for producing high-density single atoms on suitably tailored supporting matrixes hinders their industrial applications. Here, a rapid melt-quenching strategy with high throughput to synthesize single atoms with high metal-atom loadings of up to 9.7 wt% or 2.6 at% on nanoporous metal compounds is reported, representing several-fold improvements compared to benchmarks in the literature. Mechanism characterizations reveal that the high-temperature melting provides the essential liquid environment and activation energy to achieve the atomization of metals, while the following rapid-quenching pins the isolated metal atoms and stabilizes the coordination environment. In comparison with carbon-supported single-atom catalysts, various collaboration combinations of single atoms and nanoporous metal compounds can be synthesized using the strategy, thus achieving efficient hydrazine oxidation-assisted H

Atomically dispersed transition metals on carbon-based aromatic substrates are an emerging class of electrocatalysts for the electroreduction of CO2. However, electron delocalization of the metal site with the carbon support via d-π conjugation strongly hinders CO2 activation at the active metal centers. Herein, we introduce a strategy to attenuate the d-π conjugation at single Ni atomic sites by functionalizing the support with cyano moieties. In situ attenuated total reflection infrared spectroscopy and theoretical calculations demonstrate that this strategy increases the electron density around the metal centers and facilitates CO2 activation. As a result, for the electroreduction of CO2 to CO in aqueous KHCO3 electrolyte, the cyano-modified catalyst exhibits a turnover frequency of ~22,000 per hour at −1.178 V versus the reversible hydrogen electrode (RHE) and maintains a Faradaic efficiency (FE) above 90% even with a CO2 concentration of only 30% in an H-type cell. In a flow cell under pure CO2 at −0.93 V versus RHE the cyano-modified catalyst enables a current density of −300 mA/cm2 with a FE above 90%.

As a DNA receptor in the cytoplasm,cyclic GMP-AMP synthase (cGAS) can recognize abnormal DNA in the cytoplasm and activate stimulator of interferon genes (STING) to regulate the immune response. The recent studies have demonstrated that this pathway plays a role in non-infectious inflammatory diseases by promoting the expression of type Ⅰ interferon and interferon-stimulated gene.This article reviews the activation and regulation of cGAS-STING pathway in multiple systems and the effect of this pathway on the occurrence and progression of non-infectious inflammatory diseases,providing theoretical reference for future application of cGAS-STING pathway-related drugs in non-infectious inflammatory diseases.

Electrochemical CO2 reduction provides a promising strategy to product value-added fuels and chemical feedstocks. However, it remains a grand challenge to further reduce the overpotentials and increase current density for large-scale applications. Here, spontaneously Sn doped Bi/BiOx nanowires (denoted as Bi/Bi(Sn)Ox NWs) with a core-shell structure were synthesized by an electrochemical dealloying strategy. The Bi/Bi(Sn)Ox NWs exhibit impressive formate selectivity over 92% from -0.5 to -0.9 V versus reversible hydrogen electrode (RHE) and achieve a current density of 301.4 mA cm-2 at -1.0 V vs RHE. In-situ Raman spectroscopy and theoretical calculations reveal that the introduction of Sn atoms into BiOx species can promote the stabilization of the *OCHO intermediate on the Bi(Sn)Ox surface and suppress the competitive H2/CO production. This work provides effective in situ construction of the metal/metal oxide hybrid composites with heteroatom doping and new insights in promoting electrochemical CO2 conversion into formate for practical applications.

Gemcitabine-cisplatin (GP) chemotherapy is the standard first-line systemic treatment for recurrent or metastatic nasopharyngeal carcinoma (RM-NPC). In this international, double-blind, phase 3 trial (ClinicalTrials.gov identifier: NCT03581786), 289 patients with RM-NPC and no previous chemotherapy for recurrent or metastatic disease were randomized (1/1) to receive either toripalimab, a monoclonal antibody against human programmed death-1 (PD-1), or placebo in combination with GP every 3 weeks for up to six cycles, followed by monotherapy with toripalimab or placebo. The primary endpoint was progression-free survival (PFS) as assessed by a blinded independent review committee according to RECIST v.1.1. At the prespecified interim PFS analysis, a significant improvement in PFS was detected in the toripalimab arm compared to the placebo arm: median PFS of 11.7 versus 8.0 months, hazard ratio (HR) = 0.52 (95% confidence interval (CI): 0.36–0.74), P = 0.0003. An improvement in PFS was observed across key subgroups, including PD-L1 expression. As of 18 February 2021, a 40% reduction in risk of death was observed in the toripalimab arm compared to the placebo arm (HR = 0.603 (95% CI: 0.364–0.997)). The incidence of grade ≥3 adverse events (AEs) (89.0 versus 89.5%), AEs leading to discontinuation of toripalimab/placebo (7.5 versus 4.9%) and fatal AEs (2.7 versus 2.8%) was similar between the two arms; however, immune-related AEs (39.7 versus 18.9%) and grade ≥3 infusion reactions (7.5 versus 0.7%) were more frequent in the toripalimab arm. In conclusion, the addition of toripalimab to GP chemotherapy as a first-line treatment for patients with RM-NPC provided superior PFS compared to GP alone, and with a manageable safety profile. Interim analysis from the randomized phase 3 JUPITER-02 trial shows that the addition of anti-PD-1 toripalimab to standard gemcitabine/cisplatin as a first-line treatment for patients with recurrent or metastatic nasopharyngeal carcinoma has manageable toxicity and improves progression-free survival, suggesting a potential new treatment standard in this setting.

The neutralization of strongly alkaline pH conditions and acceleration of mineral weathering in alkaline Fe ore tailings have been identified as key prerequisites for eco-engineering tailings-soil formation for sustainable mine site rehabilitation. Acidithiobacillus ferrooxidans has great potential in neutralizing alkaline pH and accelerating primary mineral weathering in the tailings but little information is available. This study aimed to investigate the colonization of A. ferrooxidans in alkaline Fe ore tailings and its role in elemental sulfur (S0) oxidation, tailings neutralization, and Fe-bearing mineral weathering through a microcosm experiment. The effects of biological S0 oxidation on the weathering of alkaline Fe ore tailings were examined via various microspectroscopic analyses. It is found that (1) the A. ferrooxidans inoculum combined with the S0 amendment rapidly neutralized the alkaline Fe ore tailings; (2) A. ferrooxidans activities induced Fe-bearing primary mineral (e.g., biotite) weathering and secondary mineral (e.g., ferrihydrite and jarosite) formation; and (3) the association between bacterial cells and tailings minerals were likely facilitated by extracellular polymeric substances (EPS). The behavior and biogeochemical functionality of A. ferrooxidans in the tailings provide a fundamental basis for developing microbial-based technologies toward eco-engineering soil formation in Fe ore tailings.

Artificial photosynthesis offers a promising strategy to produce hydrogen peroxide (H2O2)—an environmentally friendly oxidant and a clean fuel. However, the low activity and selectivity of the two-electron oxygen reduction reaction (ORR) in the photocatalytic process greatly restricts the H2O2 production efficiency. Here we show a robust antimony single-atom photocatalyst (Sb-SAPC, single Sb atoms dispersed on carbon nitride) for the synthesis of H2O2 in a simple water and oxygen mixture under visible light irradiation. An apparent quantum yield of 17.6% at 420 nm together with a solar-to-chemical conversion efficiency of 0.61% for H2O2 synthesis was achieved. On the basis of time-dependent density function theory calculations, isotopic experiments and advanced spectroscopic characterizations, the photocatalytic performance is ascribed to the notably promoted two-electron ORR by forming μ-peroxide at the Sb sites and highly concentrated holes at the neighbouring N atoms. The in situ generated O2 via water oxidation is rapidly consumed by ORR, leading to boosted overall reaction kinetics. Hydrogen peroxide is an interesting target for artificial photosynthesis, although its actual production via the two-electron oxygen reduction reaction remains limited. Now, a carbon nitride-supported antimony single atom photocatalyst has been developed with a superior performance for this process.

Two novel coordination polymers (where Cu for the complex 1 and the Co for the complex 2) with distinct transition metal ions containing 4-(3,5-dicarboxylphenyl)-2-methylpyridine (H2L), the pyridyl-dicarboxylic acid ligand, have been produced under the solvothermal reaction conditions, and the two compounds’ performances and architectures were also characterized. The chemical formulae determined of two complexes are respectively [Cu(L)(H2O)]·H2O (1) and [Co3(L)2Cl2(H2O)2]·2H2O (2). Complex 1 exhibits a 2D network with a (3,6)-connected kgd topology based on the dinuclear [Cu2O2] units. In complex 2, the linear trinuclear [Co3(μ-Ocarboxylate)2(COO)2Cl2] units with mixed carboxylate and μ-Cl triple bridges are cross-linked by the L ligands into a 3D framework with a (3,6)-connected rtl topology. The complexes’ magnetic performances reflected that between consecutive metal ions, there exists the antiferromagnetic coupling. Their treatment activities on Alzheimer’s disease (AD) via focused high-intensity ultrasound were evaluated. Firstly, the Annexin V-fluorescein isothiocyanate/propidium iodide staining was implemented for the assessment of the apoptotic neurons percentage after compounds treatment. Next, the Aβ accumulation in the neurons was also detected via employing the western blotting assay.

Chlorogenic acid (CGA) is a potential inhibitor of Coronavirus Disease 2019 (COVID-19). ACE2 and its co-expressed proteins are SARS-CoV-2 receptors, which have been linked to SARS-CoV-2 infection and considered as the key target of SARS-CoV-2 in entering target cells. Here, network pharmacology was used to investigate the mechanism by which CGA affected COVID-19. A total of 70 potential targets related to the treatment of COVID-19 were obtained, among which NFE2L2, PPARG, ESR1, ACE, IL6, and HMOX1 might be the main potential targets. Finally, CGA and potential target proteins were scored by molecular docking, and the prediction results of network pharmacology were preliminarily verified. Moreover, CGA had potential anti-SARS-CoV-2 activity via integrating three common receptors in clinical practice compared with clinical trial drugs registered for the treatment of COVID-19, as shown by molecular docking. The mechanism of CGA against COVID-19 was initially investigated using network pharmacology, followed by molecular docking.

Modulation of bimetallic nanocatalysts with atomic precision would allow for significant increases in catalyst activity through the optimization of heteroatomic interplay. In practice, this level o...

Electrosynthesis of hydrogen peroxide (H

The present study explored the differences in active ingredients and in vitro anti-inflammatory effects of the decoction pieces by integrated processing(IPDP) and traditional processing(TPDP) of Polygoni Cuspidati Rhizoma et Radix(PCRER).The content of polydatin, resveratrol, emodin-8-O-β-D-glucoside, emodin, and physcion in IPDP and TPDP was determined by high-performance liquid chromatography(HPLC).The inflammation model was induced by lipopolysaccharide(LPS) in RAW264.7 cells.The mRNA levels of inflammatory cytokines tumor necrosis factor-α(TNF-α), interleukin-6(IL-6), and interleukin-1β(IL-1β) in 60% ethanol extracts of IPDP and TPDP of different concentrations(5 and 10 μg·mL~(-1)) were determined by PCR.The results showed that the content of polydatin and emodin-8-O-β-D-glucoside in IPDP was significantly higher than that in TPDP, while the content of resveratrol, emodin, and physcion was higher in TPDP.The anti-inflammatory results showed that ethanol extracts of IPDP of different concentrations(5 and 10 μg·mL~(-1)) significantly inhibited the increase in the mRNA levels of IL-1β and TNF-α induced by LPS, whereas TPDP only had a significant inhibitory effect on IL-1β.This study preliminarily showed that the total content of five active ingredients in IPDP was higher than that in TPDP, and IPDP was superior to TPDP in anti-inflammatory activity in vitro, which provided an experimental basis for the production and application of IPDP.

Pioneer plants play an important role in eco-engineering Fe ore tailings into soil for sustainable mine site rehabilitation. However, root-driven mineral weathering and secondary mineral formation remain poorly understood in tailings, despite being prerequisites for aggregate formation and pedogenesis. The present study aimed at characterizing the direct role of plant roots in tailing mineral weathering and secondary mineral formation in a compartmented cultivation system. It was found that root activities accelerated the weathering of biotite-like minerals via Fe(II) oxidation coupled with Fe(III) and Si dissolution. Numerous nanosized Fe–Si short-range-ordered (SRO) minerals and vermiculite were neoformed in the tailings after root interactions, as revealed by various microspectroscopic analyses. The Fe–Si-SRO minerals may have resulted from co-precipitation of dissolved Fe(III) and Si on mineral surfaces under alkaline and circumneutral pH conditions. Among the three plant species, Sorghum spp. (Gramineae plant) root developed most extensively in the tailings, possibly leading to more efficient mineral weathering and secondary mineral formation than Atriplex amnicola (halophyte plant) and Acacia chisholmii (leguminous plant). Overall, the study has elucidated the rhizosphere effects on tailing mineral (biotite dominant) weathering and secondary Fe–Si mineral formation, justifying pioneer plant roles in eco-engineering Fe ore tailings into soil.

Ni-rich high-energy-density lithium ion batteries pose great risks to safety due to internal short circuits and overcharging; they also have poor performance because of cation mixing and disordering problems. For Ni-rich layered cathodes, these factors cause gas evolution, the formation of side products, and life cycle decay. In this study, a new cathode electrolyte interphase (CEI) for Ni2+ self-oxidation is developed. By using a branched oligomer electrode additive, the new CEI is formed and prevents the reduction of Ni3+ to Ni2+ on the surface of Ni-rich layered cathode; this maintains the layered structure and the cation mixing during cycling. In addition, this new CEI ensures the stability of Ni4+ that is formed at 100% state of charge in the crystal lattice at high temperature (660 K); this prevents the rock-salt formation and the over-reduction of Ni4+ to Ni2+. These findings are obtained using in situ X-ray absorption spectroscopy, operando X-ray diffraction, operando gas chromatography-mass spectroscopy, and X-ray photoelectron spectroscopy. Transmission electron microscopy reveals that the new CEI has an elliptical shape on the material surface, which is approximately 100 nm in length and 50 nm in width, and covers selected particle surfaces. After the new CEI was formed on the surface, the Ni2+ self-oxidation gradually affects from the surface to the bulk of the material. It found that the bond energy and bond length of the Ni-O are stabilized, which dramatically inhibit gas evolution. The new CEI is successfully applied in a Ni-rich layered compound, and the 18650- and the punch-type full cells are fabricated. The energy density of the designed cells is up to 300 Wh/kg. Internal short circuit and overcharging safety tests are passed when using the standard regulations of commercial evaluation. This new CEI technology is ready and planned for future applications in electric vehicle and energy storage.

A facile, green and economical preparation technique is critical for the cost-effective scale-up manufacture and optoelectronic device engineering of halide perovskites. Herein, we developed a viable solvent-free mechanochemical synthetic route to systematically prepare organic–inorganic hybrid perovskites. In this work, an enormous halide library comprising 16 zero-dimensional hybrid manganese halides with the formula of AnMnX4 (A = organic cations, X = Cl, Br, n =1, 2) was synthesized through an economically and environmentally friendly mechanical grinding solid-state reaction within a quite fast time of 40 s and 100% yield. Even without any crystallization process, these AnMnX4 display strong green light emissions with the highest photoluminescence quantum yield (PLQY) of 79.5%, which reaches up to the top rank of green-light-emitting halide perovskites. Moreover, the enormous structural library facilitates us to build up a direct correlation between intermolecular Mn⋯Mn distances and PLQY, which provides a feasibility of fine-tuning luminescence performance by reasonably managing organic species to tailor the Mn⋯Mn distance. This work not only paves a green assembly way of hybrid perovskite materials but also provides a generalized method to rationally optimize the luminescence performances of hybrid manganese halides, which is potentially extended to all emissive hybrid metal halides.

The electrochemical reduction of CO2 to an ethanol product is regarded as a highly promising route for CO2 utilization. However, the poor selectivity is still a critical challenge for increasing the yield of the specific ethanol. As a CO2 reduction catalyst, the hierarchically nanoporous copper integrated with vanadium oxide can achieve a 30.1% faradaic efficiency for CO2-to-ethanol production and an ethanol partial current density of −16 mA cm−2 at −0.62 V vs. RHE, corresponding to a 4-fold increase in activity compared to bare nanoporous Cu. It even delivers an ethanol partial current density that exceeds −39 mA cm−2 at −0.8 V vs. RHE in a flow-cell reactor. The hierarchically nanoporous Cu skeleton not only facilitates both electron and electrolyte transport but also provides a large specific surface area for high active site density. Density functional theory reveals that the vanadium oxide decorated Cu surface can facilitate water dissociation and optimize the hydrogen adsorption energy on Cu, lowering the energy barrier for the protonation of carbon dioxide and C–C coupling. Meanwhile, it can increase hydrogen proton coverage on the catalyst surface and inhibit dehydration, which are beneficial for breaking the CC bond of the *HCCOH intermediate, thus enhancing the faradaic efficiency of ethanol significantly. The highly efficient conversion of CO2 to ethanol demonstrates that the hybrid electrocatalyst is considered as a promising candidate for practical electrocatalytic CO2RR applications.

To retrospectively analyze the risk factors and the prognosis according to the number of lymph node metastases (LNMs) in different neck compartments in papillary thyroid carcinoma (PTC) patients. In total, 962 patients with PTC were enrolled in this study. According to the methods of the 2015 American Thyroid Association, the treatment response of the patients was divided into a good prognosis and a poor prognosis. First, their clinical characteristics were summarized. Then, according to whether they had LNMs and the number of LNMs in different neck compartments, their risk factors and their prognosis were analyzed. Male sex, younger ( 4. Male sex, younger age, higher sTg levels and ETE were correlated with LNM > 4. Furthermore, the cutoffs for a poor prognosis of central lymph node metastasis (CLNM), lateral lymph node metastasis (LLNM) and CLNM + LLNM were > 6, > 1 and > 5, respectively. Younger age and ETE were strongly correlated with CLNM > 6. Male sex, younger age, higher sTg levels and ETE were correlated with LLNM > 1. Younger age, ETE and higher sTg levels were correlated with CLNM + LLNM > 5. Further analysis revealed a positive correlation between CLNM and LLNM. We should pay more attention to LNMs in PTC patients who are male, are of a younger age, have ETE, T1 staging and have higher sTg levels. The neck regional LNMs should be correctly evaluated to guide the surgical options for the neck LNMs in PTC. When the number of LNMs in different neck compartments has exceeded the cutoff value, they can be considered as predictors of the outcome of 131I treatment.

As a promising energy technology, the rechargeable aqueous Ni//Bi battery is attracting increasing attention. However, a suitable Bi electrode with high capacity remains elusive and its redox dynamics remain to be uncovered. Here, we report a porous metallic Bi electrode for an efficient Ni//Bi battery by the chemical dealloying method. The as-prepared porous Bi electrode delivers a capacity of 9.43 mA h cm−2 (155.8 mA h g−1) at 10 mA cm−2, with significantly improved interface charge exchange and outstanding electrochemical response compared with a bulk Bi electrode. An Ni//Bi battery based on the self-standing anode achieves an ultrahigh high area specific capacity of 5.72 mA h cm−2 with specific energy density of 4.70 mW h cm−2. Operando X-ray absorption spectroscopy, semi-operando X-ray photoelectron spectroscopy and Raman spectroscopy uncover the asymmetric redox dynamics of the Bi electrode. The present work highlights the importance of both intrinsic material properties and structural design, and will inspire more designs for high-performance electrodes of energy devices.

Summary The lack of model single-atom catalysts (SACs) and atomic-resolution operando spectroscopic techniques greatly limits our comprehension of the nature of catalysis. Herein, based on the designed model single-Fe-atom catalysts with well-controlled microenvironments, we have explored the exact structure of catalytic centers and provided insights into a spin-crossover-involved mechanism for oxygen reduction reaction (ORR) using operando Raman, X-ray absorption spectroscopies, and the developed operando 57Fe Mossbauer spectroscopy. In combination with theoretical studies, the N-FeN4C10 moiety is evidenced as a more active site for ORR. Moreover, the potential-relevant dynamic cycles of both geometric structure and electronic configuration of reactive single-Fe-atom moieties are evidenced via capturing the peroxido (∗O2−) and hydroxyl (∗OH−) intermediates under in situ ORR conditions. We anticipate that the integration of operando techniques and SACs in this work shall shed some light on the electronic-level insight into the catalytic centers and underlying reaction mechanism.

A general graphene quantum dot-tethering design strategy to synthesize single-atom catalysts (SACs) is presented. The strategy is applicable to different metals (Cr, Mn, Fe, Co, Ni, Cu, and Zn) and supports (0D carbon nanosphere, 1D carbon nanotube, 2D graphene nanosheet, and 3D graphite foam) with the metal loading of 3.0-4.5 wt %. The direct transmission electron microscopy imaging and X-ray absorption spectra analyses confirm the atomic dispersed metal in carbon supports. Our study reveals that the abundant oxygenated groups for complexing metal ions and the rich defective sites for incorporating nitrogen are essential to realize the synthesis of SACs. Furthermore, the carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO2 reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications.