Reference intervals of Cyfra21-1 and CEA in healthy adult Han Chinese population.

Objective: This study aimed to establish the reference intervals of Cyfra21-1 and CEA for the local screening populations using a chemiluminescence method. Methods: A total of 4845 healthy adults and 190 lung cancer patients were included from the First Hospital of Hebei Medical University. The levels of Cyfra21-1 and CEA were measured to establish the local reference intervals. Results: The upper limit reference intervals for Cyfra21-1 and CEA were determined as 3.19 ng/ml and 3.13 ng/ml, respectively. Notably, both Cyfra21-1 and CEA levels were found to be higher in males than in females. Additionally, both biomarkers showed an increasing trend with age.In terms of diagnostic efficacy, the receiver operating characteristic (ROC) curve areas for Cyfra21-1, CEA, and their combination in lung cancer were 0.86, 0.73, and 0.91, respectively. Conclusion: Our study revealed that the reference intervals of Cyfra21-1 and CEA in the local population differed from the established reference intervals. Furthermore, both biomarkers exhibited gender-dependent variations and demonstrated a positive correlation with age. Combining the two biomarkers showed potential for improving the diagnosis rate of lung cancer.

Application of Thermal Cycling Amplification Chip Method in the Detection of Respiratory Machine-Associated Pneumonia Pathogens.

Objective: Investigating the application effectiveness of using loop-mediated isothermal amplification (LAMP) on a microfluidic chip to detect the pathogens associated with ventilator-associated pneumonia (VAP). Methods: Eighty samples of bronchoalveolar lavage fluid from patients with ventilator-associated pneumonia (VAP) were collected at The First Hospital of Hebei Medical University from July 2022 to July 2023. The bacterial culture technique and the LAMP method were used to detect the nucleic acid of the pathogens in the patient samples. The positivity rates of bacterial culture and LAMP method in detecting VAP pathogens were analyzed. Results: A total of 80 specimens were examined, with 73 positive specimens detected using the LAMP method (positivity rate of 91.25%) and 60 positive specimens detected using bacterial culture (positivity rate of 75.00%). The LAMP method exhibited a higher number of positive detections compared to bacterial culture. Both methods showed a high level of concordance and were virtually identical in detecting methicillin-resistant Staphylococcus aureus, Staphylococcus aureus, Escherichia coli, Pseudomonas aeruginosa, Enterobacter aerogenes, Haemophilus influenzae, and Streptococcus pneumoniae. Conclusion: The LAMP method demonstrates significantly improved performance in the detection of pathogens for VAP, with a higher pathogen positivity rate compared to bacterial culture. This method holds promising prospects for clinical application.

Breaking solvation dominance of ethylene carbonate via molecular charge engineering enables lower temperature battery.

Low temperatures severely impair the performance of lithium-ion batteries, which demand powerful electrolytes with wide liquidity ranges, facilitated ion diffusion, and lower desolvation energy. The keys lie in establishing mild interactions between Li+ and solvent molecules internally, which are hard to achieve in commercial ethylene-carbonate based electrolytes. Herein, we tailor the solvation structure with low-ε solvent-dominated coordination, and unlock ethylene-carbonate via electronegativity regulation of carbonyl oxygen. The modified electrolyte exhibits high ion conductivity (1.46 mS·cm-1) at -90 °C, and remains liquid at -110 °C. Consequently, 4.5 V graphite-based pouch cells achieve ~98% capacity over 200 cycles at -10 °C without lithium dendrite. These cells also retain ~60% of their room-temperature discharge capacity at -70 °C, and miraculously retain discharge functionality even at ~-100 °C after being fully charged at 25 °C. This strategy of disrupting solvation dominance of ethylene-carbonate through molecular charge engineering, opens new avenues for advanced electrolyte design.

A biocompatible electrolyte enables highly reversible Zn anode for zinc ion battery.

Progress towards the integration of technology into living organisms requires power devices that are biocompatible and mechanically flexible. Aqueous zinc ion batteries that use hydrogel biomaterials as electrolytes have emerged as a potential solution that operates within biological constraints; however, most of these batteries feature inferior electrochemical properties. Here, we propose a biocompatible hydrogel electrolyte by utilising hyaluronic acid, which contains ample hydrophilic functional groups. The gel-based electrolyte offers excellent anti-corrosion ability for zinc anodes and regulates zinc nucleation/growth. Also, the gel electrolyte provides high battery performance, including a 99.71% Coulombic efficiency, over 5500 hours of long-term stability, improved cycle life of 250 hours under a high zinc utilization rate of 80%, and high biocompatibility. Importantly, the Zn//LiMn2O4 pouch cell exhibits 82% capacity retention after 1000 cycles at 3 C. This work presents a promising gel chemistry that controls zinc behaviour, offering great potential in biocompatible energy-related applications and beyond.

Polymeric Carbon Nitride with Chirality Inherited from Supramolecular Assemblies.

The facile synthesis of chiral materials is of paramount importance for various applications. Supramolecular preorganization of monomers for thermal polymerization has been proven as an effective tool to synthesize carbon and carbon nitride-based (CN) materials with ordered morphology and controlled properties. However, the transfer of an intrinsic chemical property, such as chirality from supramolecular assemblies to the final material after thermal condensation, was not shown. Here, we report the large-scale synthesis of chiral CN materials capable of enantioselective recognition. To achieve this, we designed supramolecular assemblies with a chiral center that remains intact at elevated temperatures. The optimized chiral CN demonstrates an enantiomeric preference of ca. 14 %; CN electrodes were also prepared and show stereoselective interactions with enantiomeric probes in electrochemical measurements. By adding chirality to the properties transferrable from monomers to the final product of a thermal polymerization, this study confirms the potential of using supramolecular precursors to produce carbon and CN materials and electrodes with designed chemical properties.

B-/Si-containing electrolyte additive efficiently establish a stable interface for high-voltage LiCoO2 cathode and its synergistic effect on LiCoO2/graphite pouch cells.

An effective electrolyte additive, 3-(tert-Butyldimethylsilyoxy) phenylboronic acid (TBPB), is proposed to significantly improve the cycle stability of high voltage LiCoO2 (LCO) cathode. Experimental and computational results show that TBPB has a relatively higher oxidation activity than base electrolyte, and preferentially constructs a stable cathode electrolyte interphase (CEI) containing B-/Si- components on LCO surface. Theoretical calculation, XPS and NMR data show that TBPB-derived CEI layer contains B-F species and has the function of eliminating HF. The as-formed CEI effectively inhibits the detrimental side reactions from electrolyte decomposition and LCO surface structure reconstruction. The capacity retention of LCO/Li half-cell increases from 38.92% (base electrolyte) to 83.70% after 150 cycles at 1 C between 3.0 V and 4.5 V by adding 1% TBPB. Moreover, TBPB is also reduced prior to base electrolyte, forming an ionic conducting solid electrolyte interphase (SEI) on graphite surface. Benefiting from the synergistic effect between CEI layer on LCO cathode and SEI layer on graphite anode to effectively decrease the electrolyte decomposition, the capacity retention of commercial LCO/graphite pouch cell with 1% TBPB increases from 10.44% to 76.13% after 400 cycles at 1 C between 3.0 V and 4.5 V. This work demonstrates that TBPB can act as an effective film-forming additive for high energy density LCO cathode at high voltage, and provides novel insights for its commercial application from the aspect of synergistically interfacial stability.

The Origin of Solvent Deprotonation in LiI-added Aprotic Electrolytes for Li-O2 Batteries.

LiI and LiBr have been employed as soluble redox mediators (RMs) in electrolytes to address the sluggish oxygen evolution reaction kinetics during charging in aprotic Li-O2 batteries. Compared to LiBr, LiI exhibits a redox potential closer to the theoretical one of discharge products, indicating a higher energy efficiency. However, the reason for the occurrence of solvent deprotonation in LiI-added electrolytes remains unclear. Here, by combining ab initio calculations and experimental validation, we find that it is the nucleophile I O 3 - ${{{\rm I}{\rm O}}_{3}^{-}}$ that triggers the solvent deprotonation and LiOH formation via nucleophilic attack, rather than the increased solvent acidity or the elongated C-H bond as previously suggested. As a comparison, the formation of B r O 3 - ${{{\rm B}{\rm r}{\rm O}}_{3}^{-}}$ in LiBr-added electrolytes is found to be thermodynamically unfavorable, explaining the absence of LiOH formation. These findings provide important insight into the solvent deprotonation and pave the way for the practical application of LiI RM in aprotic Li-O2 batteries.

Developing extended visible light responsive polymeric carbon nitrides for photocatalytic and photoelectrocatalytic applications.

Polymeric carbon nitride (CN) has emerged as an attractive material for photocatalysis and photoelectronic devices. However, the synthesis of porous CNs with controlled structural and optical properties remains a challenge, and processable CN precursors are still highly sought after for fabricating homogenous CN layers strongly bound to a given substrate. Here, we report a general method to synthesize highly dispersed porous CN materials that show excellent photocatalytic activity for the hydrogen evolution reaction and good performance as photoanodes in photoelectrochemical cells (PEC): first, supramolecular assemblies of melem and melamine in ethylene glycol and water are prepared using a hydrothermal process. These precursors are then calcined to yield a water-dispersible CN photocatalyst that exhibits beneficial charge separation under illumination, extended visible-light response attributed to carbon doping, and a large number of free amine groups that act as preferential sites for a Pt cocatalyst. The optimized CN exhibits state-of-the-art HER rates up to 23.1 mmol h-1 g-1, with an AQE of 19.2% at 395 nm. This unique synthetic route enables the formation of a homogeneous precursor paste for substrate casting; consequently, the CN photoanode exhibits a low onset potential, a high photocurrent density and good stability after calcination.

A diagnostic test of real-time PCR detection in the diagnosis of clinical bloodstream infection.

BACKGROUND: Blood culture remains the standard for diagnosing bloodstream infections, but it is difficult to identify bacteria directly and timeliness. The real-time polymerase chain reaction (PCR) has the potential to fill this diagnostic gap. This study intends to explore the sensitivity and specificity of PCR in detecting bloodstream infection pathogens and to compare it with routine blood culture to explore its clinical application value. METHODS: A total of 126 patients with bloodstream infections collected from various clinical departments of The First Hospital of Hebei Medical University. The patient's sample was divided into two parts. The one for multiplex PCR detection was performed using the Pathogeno Elite Multiplex PCR kit. Another blood culture was a fully automatic blood culture system from Autobio company. RESULTS: Among the 126 patients, a total of 17 pathogens were detected by PCR and blood culture both methods. PCR detected a total of 43 positive samples and 83 negative samples. Five samples were positive with blood culture, and 81 were negative. The negative predictive value of PCR was 0.98, with a sensitivity of 0.71 and a specificity of 0.68. A total of 38 specimens were positive for PCR but negative for blood culture, and 2 samples were positive for blood culture but negative for PCR. The top 5 pathogens with PCR detection were Epstein-Barr virus (27 cases), Human herpes virus 5 (9 cases), Klebsiella pneumoniae (5 cases), Staphylococcus (5 cases), and Stenotrophomonas maltophilia (4 cases). CONCLUSIONS: PCR detection can rapidly identify more pathogens and even multi-pathogen infections. Therefore, PCR testing may improve pathogen detection in patients with suspected bloodstream infections, enabling targeted treatment of patients.

Insight into the Contribution of Nitriles as Electrolyte Additives to the Improved Performances of the LiCoO2 Cathode.

Nitriles have been successfully used as electrolyte additives for performance improvement of commercialized lithium-ion batteries based on the LiCoO2 cathode, but the underlying mechanism is unclear. In this work, we present an insight into the contribution of nitriles via experimental and theoretical investigations, taking for example succinonitrile. It is found that succinonitrile can be oxidized together with PF6- preferentially on LiCoO2 compared to the solvents in the electrolyte, making it possible to avoid the formation of hydrogen fluoride from the electrolyte oxidation decomposition, which is detrimental to the LiCoO2 cathode. Additionally, inorganic LiF and -NH group-containing polymers are formed from the preferential oxidation of succinonitrile, constructing a protective interphase on LiCoO2, which suppresses electrolyte oxidation decomposition and prevents LiCoO2 from structural deterioration. Consequently, the LiCoO2 cathode presents excellent stability under cycling and storing at high voltages.

Construction of Low-Impedance and High-Passivated Interphase for Nickel-Rich Cathode by Low-Cost Boron-Containing Electrolyte Additive.

The nickel-rich cathode LiNi0.8 Co0.1 Mn0.1 O2 (NCM811) possesses the advantages of high reversible specific capacity and low cost, thus regarded as a promising cathode material for lithium-ion batteries (LIBs). However, the capacity of the NCM811 decays rapidly at high voltage due to the extremely unstable electrode/electrolyte interphase. The discharge capability at low temperature is also impaired because of the increasing interfacial impedance. Herein, a low-cost film-forming electrolyte additive with multi-function, phenylboronic acid (PBA), was employed to modify the interphasial properties of the NCM811 cathode. Theoretical calculation and experimental results showed that PBA constructed a highly conductive and steady cathode electrolyte interphase (CEI) film through preferential oxidation decomposition, which greatly improved the interfacial properties of the NCM811 cathode at room (25 °C) and low temperature (-10 °C). Specifically, the capacity retention of NCM811/Li cell was increased from 68 % to 87 % after 200 cycles with PBA additive. Moreover, the NCM811/Li cell with PBA additive delivered higher discharge capacity under -10 °C at 0.5 C (173.7 mAh g-1 vs. 111.1 mAh g-1 ). Based on the improvement of NCM811 interphasial properties by additive PBA, the capacity retention of NCM811/graphite full-cell was enhanced from 49 % to 65 % after 200 cycles.

Cost-Efficient Film-Forming Additive for High-Voltage Lithium-Nickel-Manganese Oxide Cathodes.

The operating voltage of lithium-nickel-manganese oxide (LiNi0.5Mn1.5O4, LNMO) cathodes far exceeds the oxidation stability of the commercial electrolytes. The electrolytes undergo oxidation and decomposition during the charge/discharge process, resulting in the capacity fading of a high-voltage LNMO. Therefore, enhancing the interphasial stability of the high-voltage LNMO cathode is critical to promoting its commercial application. Applying a film-forming additive is one of the valid methods to solve the interphasial instability. However, most of the proposed additives are expensive, which increases the cost of the battery. In this work, a new cost-efficient film-forming electrolyte additive, 4-trifluoromethylphenylboronic acid (4TP), is adopted to enhance the long-term cycle stability of LNMO/Li cell at 4.9 V. With only 2 wt % 4TP, the capacity retention of LNMO/Li cell reaches up to 89% from 26% after 480 cycles. Moreover, 4TP is effective in increasing the rate performance of graphite anode. These results show that the 4TP additive can be applied in high-voltage LIBs, which significantly increases the manufacturing cost while improving the battery performance.

A Novel Electrolyte Additive Enables High-Voltage Operation of Nickel-Rich Oxide/Graphite Cells.

Nickel-rich oxide/graphite cells under high voltage operation provide high energy density but present short cycle life because of the parasitic electrolyte decomposition reactions. In this work, we report a novel electrolyte additive, N,O-bis(trimehylsilyl)-trifluoroacetamide (NOB), which enables nickel-rich oxide/graphite cells to operate stably under high voltage. When evaluated in a nickel-rich oxide-based full cell, LiNi0.5Co0.2Mn0.3O2 (NCM523)/graphite using a carbonate electrolyte, 1 wt % NOB provides the cell with capacity retention improved from 38% to 73% after 100 cycles at 1C under 4.5 V. It is found that NOB is able to eliminate hydrogen fluoride in the electrolyte. The radicals resulting from the interaction of NOB with the fluoride ion can be preferentially oxidized on the cathode compared with the electrolyte solvents, with its reaction products constructing N-containing interphases simultaneously on the cathode and anode, which suppress the parasitic electrolyte decomposition reactions, leading to the significantly improved cycle stability of nickel-rich oxide/graphite cells under high voltage.

Highly Efficient Polymeric Carbon Nitride Photoanode with Excellent Electron Diffusion Length and Hole Extraction Properties.

Polymeric carbon nitride (CN) has emerged as a promising semiconductor in photoanodes for photoelectrochemical cells (PECs) owing to its suitable electronic structure, tunable band gap, high stability, and low price. However, the poor electron diffusion within the CN layer and hole extraction to the solution still limit its applicability in PECs. Here, we report the fabrication of a CN photoanode with excellent electron diffusion length and remarkable hole extraction properties by careful design of its electronic interfaces. We combine complementary synthetic approaches to grow tightly packed CN layers forming a type-II heterojunction, which results in a CN photoanode with excellent charge separation, high electronic conductivity, and remarkable hole extraction efficiency. The optimized CN photoanode displays excellent PEC performance, reaching up to 270 µA cm-2 in a 0.1 M KOH solution at 1.23 V vs RHE, extremely low onset potential (∼0.0012 V), and long-term stability up to 18 h.

Stabilized High-Voltage Cathodes via an F-Rich and Si-Containing Electrolyte Additive.

High-voltage cathodes provide a promising solution to the energy density limitation of currently commercialized lithium-ion batteries, but they are unstable in electrolytes during the charge/discharge process. To address this issue, we propose a novel electrolyte additive, pentafluorophenyltriethoxysilane (TPS), which is rich in elemental F and contains elemental Si. The effectiveness of TPS has been demonstrated by cycling a representative high-voltage cathode, LiNi0.5Mn1.5O4 (LNMO), in 1.0 M LiPF6-diethyl carbonate/ethylene carbonate/ethyl methyl carbonate (2/3/5 in weight). LNMO presents an increased capacity retention from 28 to 85% after 400 cycles at 1 C by applying 1 wt % TPS. Further electrochemical measurements combined with spectroscopic characterization and theoretical calculations indicate that TPS can not only construct a robust protective cathode electrolyte interphase via its oxidation during initial lithium desertion but also scavenge the detrimental hydrogen fluoride (HF) present in the electrolyte via its strong combination with the species HF, F-, and H+, highly stabilizing LNMO during the charge/discharge process. These features of TPS provide a new solution to the obstacle in the practical application of high-voltage cathodes not limited to LNMO.

Co-modified MoO2 nanoparticles highly dispersed on N-doped carbon nanorods as anode electrocatalyst of microbial fuel cells.

Cobalt-modified molybdenum dioxide nanoparticles highly dispersed on nitrogen-doped carbon nanorods (Co-MoO2/NCND), are synthesized from anilinium trimolybdate dihydrate nanorods, for the performance improvement of microbial fuel cell based on a mixed bacterial culture. Electrochemical measurements demonstrate that the as-synthesized Co-MoO2/NCND exhibits excellent electrocatalytic activity for the charge transfer on anode, providing the cell with a maximum power density of 2.06 ±â€¯0.05 W m-2, which is strikingly higher than the bare carbon felt anode (0.49 ±â€¯0.04 W m-2). The excellent performance of Co-MoO2/NCND is ascribed to the increased electronic conductivity of carbon nanorods by N-doping, the high ability of MoO2 to enrich electroactive bacteria, as demonstrated by high-throughput sequencing, and the enhanced activity of MoO2 by Co-modifying toward redox reactions in electroactive bacteria. This report provides a new concept of anode electrocatalyst fabrications for the application of microbial fuel cells in electricity generation and wastewater treatment.

Tailoring Low-Temperature Performance of a Lithium-Ion Battery via Rational Designing Interphase on an Anode.

Performances of lithium-ion batteries at subambient temperatures are extremely restricted by the resistive interphases originated from electrolyte decomposition, especially on the anode surface. This work reports a novel strategy that an anode interphase of low impedance is constructed by applying an electrolyte additive dimethyl sulfite (DMS). Electrochemical measurements indicate that the as-constructed interphase provides graphite/LiNi0.5Co0.2Mn0.3O2 pouch cells with excellent low-temperature performance, outperforming the interphase constructed by 1,3,2-dioxathiolane 2,2-dioxide (DTD), a common commercially used electrolyte additive. Spectral characterizations in combination with theoretical calculations demonstrate that the improved performance is attributed to the unique molecular structure of DMS, which presents appropriate reduction activity and constructs the more stable and ionically conductive anode interphase due to the weaker combination of its reduction product with lithium ions than DTD. This rational design of interphases via an additive structure has been proven to be a low cost but rather an effective approach to tailor the performances of lithium-ion batteries.

Understanding and Suppressing the Destructive Cobalt(II) Species in Graphite Interphase.

Co2+ species dissolved from LiCoO2 in lithium-ion batteries have been well-established to be responsible for the cell performance fading, especially when the cells are charged to high voltage or at elevated temperatures. The accepted underlying mechanism is the deposition of Co2+ on the graphite anode that destroys the interphase. In this work, we report that the dissolved Co2+ exists in the form of both Co0 and Co2+ on the graphite anode surface, while Co0 formed at lithium insertion potential can be reoxidized to Co2+ during charging. Moreover, Co0 shows a higher catalytic activity than Co2+ toward the reductive decomposition of carbonate electrolyte. An interphase of ∼4 nm was thus engineered from a film-forming additive 3-sulflone, which completely eliminates the destructive effect of the deposited Co species. The understanding of the destructive role of the dissolved Co2+ on the interphasial stability of the graphite electrode and an effective strategy to suppress such a failure mechanism provides fresh insight into the failure mechanism of manganese-based cathode chemistries, which serves as a better guideline for electrolyte design for future batteries.

Overlooked electrolyte destabilization by manganese (II) in lithium-ion batteries.

Transition-metal dissolution from cathode materials, manganese in particular, has been held responsible for severe capacity fading in lithium-ion batteries, with the deposition of the transition-metal cations on anode surface, in elemental form or as chelated-complexes, as the main contributor for such degradations. In this work we demonstrate with diverse experiments and calculations that, besides interfacial manganese species on anode, manganese(II) in bulk electrolyte also significantly destabilizes electrolyte components with its unique solvation-sheath structure, where the decompositions of carbonate molecules and hexafluorophosphate anion are catalyzed via their interactions with manganese(II). The manganese(II)-species eventually deposited on anode surface resists reduction to its elemental form because of its lower electrophilicity than carbonate molecule or anion, whose destabilization leads to sustained consumption. The reveal understanding of the once-overlooked role of manganese-dissolution in electrolytes provides fresh insight into the failure mechanism of manganese-based cathode chemistries, which serves as better guideline to electrolyte design for future batteries.

Stabilizing a High-Voltage Lithium-Rich Layered Oxide Cathode with a Novel Electrolyte Additive.

We report a novel electrolyte additive, bis(trimethylsilyl)carbodiimide, that effectively stabilizes high-voltage lithium-rich oxide cathode. Charge/discharge tests demonstrate that even trace amounts of bis(trimethylsilyl)carbodiimide in a baseline electrolyte improve the cycling stability of this cathode significantly, either in Li-based half cells or graphite-based full cells, where the capacity retention after 200 cycles between 2 and 4.8 V at 0.5C is enhanced from 40 to 72% and 49 to 77%, respectively. Analyses using physical characterization and theoretical calculations reveal that this additive not only builds a protective film on the cathode but also eliminates detrimental hydrogen fluoride via its strong coordination with hydrogen fluoride or protons.