Search

Hybrid capacitive deionization (HCDI) emerges as a burgeoning electrochemical desalination technology due to the utilization of profitable pseudocapacitive reactions. Although tunable organic compounds are potential faradaic electrode materials, their insufficient active sites and high water‐solubility restrict practical HCDI applications. Herein, a pseudocapacitive organic polymer (PNDS) is proposed with diverse redox‐active sites for electrochemical deionization. The pronounced molecular aromaticity and strong π‐electron delocalization not only endow PNDS polymer with framework rigidity, but refine its electronic structure to bolster redox activity and electron affinity. As an electrode material, the PNDS polymer demonstrates a substantial pseudocapacitive capacitance of 390 F g−1 and sustains long‐term stability at 96.3% after 5000 cycles, surpassing reported Na+‐capturing organic electrodes. In‐operando monitoring techniques and theoretical calculations reveal efficient Na+ capture at the C═N and C═O redox‐active sites within the PNDS electrode during repeated electrosorption processes. As a conceptual demonstration, a high‐performance HCDI device equipped with the PNDS electrode exhibits an impressive salt removal capacity (66.4 mg g−1), a rapid removal rate (2.2 mg g−1 min−1) and stable regeneration property. More importantly, an integrated desalination system is engineered to rapidly and repeatedly treat saltwater resources for human consumption and agricultural irrigation, highlighting its promising prospects for high‐efficiency desalination applications. [ABSTRACT FROM AUTHOR]

Electrocatalytic reduction of nitrate to ammonia provides a green alternate to the Haber–Bosch method, yet it suffers from sluggish kinetics and a low yield rate. The nitrate reduction follows a tandem reaction of nitrate reduction to nitrite and subsequent nitrite hydrogenation to generate ammonia, and the ammonia Faraday efficiency (FE) is limited by the competitive hydrogen evolution reaction. Herein, we design a heterostructure catalyst to remedy the above issues, which consists of Ni nanosphere core and Ni(OH)2 nanosheet shell (Ni/Ni(OH)2). In situ Raman spectroscopy reveals Ni and Ni(OH)2 are interconvertible according to the applied potential, facilitating the cascade nitrate reduction synergistically. Consequently, it attains superior electrocatalytic nitrate reduction performance with an ammonia FE of 98.50 % and a current density of 0.934 A cm−2 at −0.476 V versus reversible hydrogen electrode, and exhibits an average ammonia yield rate of 84.74 mg h−1 cm−2 during the 102‐hour stability test, which is highly superior to the reported catalysts tested under similar conditions. Density functional theory calculations corroborate the synergistic effect of Ni and Ni(OH)2 in the tandem reaction of nitrate reduction. Moreover, the Ni/Ni(OH)2 catalyst also possesses good capability for methanol oxidation and thus is used to establish a system coupling with nitrate reduction. [ABSTRACT FROM AUTHOR]

Due to their atomically dispersed active centers, single‐atom nanozymes (SAzymes) have unparalleled advantages in cancer catalytic therapy. Here, loaded with chlorin e6 (Ce6), a hydrothermally mass‐produced bimetallic silicate‐based nanoplatforms with atomically dispersed manganese/gadolinium (Mn/Gd) dual sites and oxygen vacancies (OVs) (PMnSAGMSNs‐V@Ce6) is constructed for tumor glutathione (GSH)‐triggered chemodynamic therapy (CDT) and O2‐alleviated photodynamic therapy. The band gaps of silica are significantly reduced from 2.78 to 1.88 eV by doping with metal ions, which enables it to be excited by a 650 nm laser to produce electron‐hole pairs, thereby facilitating the generation of reactive oxygen species. The Gd sites can modulate the local electrons of the atom‐catalyzed Mn sites, which contribute to the generation of superoxide and hydroxyl radicals (•OH). Tumor GSH‐triggered Mn2+ release can convert endogenous H2O2 to •OH and realize GSH‐depletion‐enhanced CDT. Significantly, the hydrothermally generated OVs can not only capture Mn and Gd atoms to form atomic sites but also can elongate and weaken the O‐O bonds of H2O2, thereby improving the efficacy of Fenton reactions. The degraded Mn2+/Gd3+ ions can be used as tumor‐specific magnetic resonance imaging contrast agents. All the experimental results demonstrate the great potential of PMnSAGMSNs‐V@Ce6 as cancer theranostic agent. [ABSTRACT FROM AUTHOR]

Developing high‐capacity conversion‐type anodes with superior durability substituting conventional graphite anodes is urgently desired to improve the energy density of lithium‐ion batteries (LIBs). However, fatal capacity decay during cycling of the conversion‐type anodes, which is primarily due to their inevitable structural degradation and continuous solid‐electrolyte interphase reformation induced by drastic volume change, has highly restricted their commercialization. And, the interrelated effects of phase transformation, structural evolution, and electrochemical characteristics of the conversion‐type anodes during cycling remain poorly understood. Herein, the findings on the fabrication and understanding of a previously unexplored entropy‐stabilized spinel oxide, (Co0.2Mn0.2V0.2Fe0.2Zn0.2)3O4 as a promising conversion anode for LIBs, exhibiting not only moderate volume change character but also highly reversible capacities of ≈900 mAh g−1 for 500 cycles at 0.2 A g−1 and ≈500 mAh g−1 for 2000 cycles at 3 A g−1, respectively, are reported. Evidenced by in situ transmission electron microscopy coupled with theoretical calculations, its underlying mechanism underpinning highly reversible Li storage is explicitly revealed, which originates from reversible phase transformation and domain reconstruction during cycling. Moreover, the origin of small volume change is also clearly clarified. This work provides renewed mechanistic insights into designing high‐capacity and durable conversion‐type electrode materials for high‐performance LIBs. [ABSTRACT FROM AUTHOR]

Molybdenum (Mo)‐based nanozymes have been attracting increasingly extensive attention in photocatalytic antitumor field due to their versatile physicochemical properties, whereas the limited light capture rate and high recombination rate of photogenerated carriers seriously impedes their further development. Herein, MoO3‐starring silica nanozymes with hyaluronic acid modification (HMMSNs@HA) are innovated by hydrogenation to simultaneously achieve oxygen vacancies (OVs) engineering and tumor adaptive accumulation for the second near‐infrared (NIR‐II, 1064 nm) light‐potentiated thermal‐catalytic therapy. The hydrogenation‐regulated OVs can narrow the band gap of HMMSNs from 2.66 to 1.16 eV, achieving optimal optical absorption in NIR‐II region. Additionally, HMMSNs hold high separation efficacy of electron‐hole pairs to facilitate the generation of reactive oxygen species under laser irradiation. Significantly, HMMSNs@HA are stable in tumor microenvironment, while can degrade in normal physiological conditions, thereby offering tumor‐adaptive accumulation. Synchrotron radiation‐based extended X‐ray absorption fine structure spectroscopy reveals that OVs enabling the Mo4+ and Mo5+ formation, which can react with tumor endogenous H2O2 to produce hydroxyl radicals. Furthermore, OVs‐induced localized surface plasmon resonance effect endows the nanozymes with photothermal conversion efficacy of 32.3%, which affords NIR‐II‐excited photonic hyperthermia‐enhances catalytic therapy. All the experimental results demonstrate the high safety and superiorities of HMMSNs@HA for NIR‐II‐initiate therapy. [ABSTRACT FROM AUTHOR]

Although high ionic conductivities have been achieved in most solid‐state electrolytes used in lithium metal batteries (LMBs), rapid and stable lithium‐ion transport between solid‐state electrolytes and lithium anodes remains a great challenge due to the high interfacial impedances and infinite volume changes of metallic lithium. In this work, a chemical vapor‐phase fluorination approach is developed to establish a lithiophilic surface on rubber‐derived electrolytes, which results in the formation of a resilient, ultrathin, and mechanically integral LiF‐rich layer after electrochemical cycling. The resulting ultraconformal layer chemically connects the electrolyte and lithium anode and maintains dynamic contact during operation, thus facilitating rapid and stable lithium‐ion transport across interfaces, as well as promoting uniform lithium deposition and inhibiting side reactions between electrolyte components and metallic lithium. LMBs containing the novel electrolyte have an ultralong cycling life of 2500 h and deliver a high critical current density of 1.1 mA cm−2 in lithium symmetric cells as well as showing good stability over 300 cycles in a full cell. [ABSTRACT FROM AUTHOR]

Background: The objective of this study was to evaluate the safety and efficacy of nab‐paclitaxel, trastuzumab, and pertuzumab as neoadjuvant therapy (NAT) in patients with human epidermal growth factor receptor 2 HER2+ breast cancer (HER2+ BC) to determine pathologic complete response (pCR), invasive disease‐free survival (iDFS), and overall survival. Methods: Forty‐five patients with HER2+ BC Stages II–III were to be enrolled from 2013 to 2017. Patients were treated with weekly nab‐paclitaxel (100 mg/m2 intravenously), weekly trastuzumab (4 mg/kg loading dose, then 2 mg/kg), and six cycles of pertuzumab (840 mg loading dose, then 420 mg intravenously day 1 every 21 days). Results: Median follow‐up was 60 months (95% CI, 32.3–55.6) and pCR was 29/45 (64%). The 5‐year iDFS for patients who achieved pCR (N = 29) was 96.3% (95% CI, 76.5–99.5) and non‐pCR patients (N = 16) was 74.3% (95% CI, 39.1–91.0). The 5‐year overall survival (N = 45) was 94.1% (95% CI, 77.6–98.5). Based on hormonal status, the 5‐year iDFS for HR+ pCR patients (N = 14) was 92.3% (95% CI, 56.6–98.9) and for HR− (N = 15) was 100% (p =.3). Conclusions: This anthracycline/carboplatin‐free regimen with nab‐paclitaxel achieved a pCR rate of 64% in patients with HER2+ BC. The 5‐year iDFS in patients with and without pCR was 96.3% and 74.3%, respectively. The pCR rate is comparable with docetaxel, carboplatin, trastuzumab, and pertuzumab therapy in the NAT setting, but with fewer treatment‐associated toxicities. This finding suggests the possibility of safe avoidance of anthracyclines and carboplatin as components of NAT in patients with HER2+ BC. This anthracycline/carboplatin‐free regimen with nab‐paclitaxel achieved a pathologic complete response rate of 64% in patients with human epidermal growth factor receptor 2 breast cancer (HER2+ BC). This finding suggests the possibility of safe avoidance of anthracyclines and carboplatin as components of neoadjuvant therapy in HER2+ BC patients. [ABSTRACT FROM AUTHOR]

The title compound, [Cu(4)I(4)(C(9)H(13)N)(4)], has a distorted cubane-like [Cu(4)I(4)] core structure. Each Cu(I) atom is tetra-hedrally coordinated by three I atoms and one N atom of an benzyl-dimethyl-amine ligand. Each I atom acts as a μ(3)-ligand, linking three Cu(I) atoms. The Cu-I bond distances vary between 2.6328 (7) and 2.7121 (6) Å, while the Cu-N bond distances vary between 2.107 (3) and 2.122 (3) Å.