Scalable Cathodic H2O2 Electrosynthesis using Cobalt-Coordinated Nanocellulose Electrocatalyst.

Converting hierarchical biomass structure into cutting-edge architecture of electrocatalysts can effectively relieve the extreme dependency of nonrenewable fossil-fuel-resources typically suffering from low cost-effectiveness, scarce supplies, and adverse environmental impacts. A cost-effective cobalt-coordinated nanocellulose (CNF) strategy is reported for realizing a high-performance 2e-ORR electrocatalysts through molecular engineering of hybrid ZIFs-CNF architecture. By a coordination and pyrolysis process, it generates substantial oxygen-capturing active sites within the typically oxygen-insulating cellulose, promoting O2 mass and electron transfer efficiency along the nanostructured Co3O4 anchored with CNF-based biochar. The Co-CNF electrocatalyst exhibits an exceptional H2O2 electrosynthesis efficiency of ≈510.58 mg L-1 cm-2 h-1 with an exceptional superiority over the existing biochar-, or fossil-fuel-derived electrocatalysts. The combination of the electrocatalysts with stainless steel mesh serving as a dual cathode can strongly decompose regular organic pollutants (up to 99.43% removal efficiency by 30 min), showing to be a desirable approach for clean environmental remediation with sustainability, ecological safety, and high-performance.

Hierarchical Bilayer Polyelectrolyte Ion Paper Conductor for Moisture-Induced Power Generation.

Harvesting energy from air water (atmospheric moisture) promises a sustainable self-powered system without any restrictions from specific environmental requirements (e.g., solar cells, hydroelectric, or thermoelectric devices). However, the present moisture-induced power devices traditionally generate intermittent or bursts of energy, especially for much lower current outputs (generally keeping at nA or µA levels) from the ambient environment, typically suffering from inferior ionic conductivity and poor hierarchical structure design for manipulating sustained air water and ion-charge transport. Here, we demonstrate a universal strategy to design a high-performance bilayer polyelectrolyte ion paper conductor for generating continuous electric power from ambient humidity. The generator can produce a continuous voltage of up to 0.74 V and also an exceptional current of 5.63 mA across a single 1.0 mm-thick ion paper conductor. We discover that the sandwiched LiCl-nanocellulose-engineered paper promises an ion-transport junction between the negatively and positively charged bilayer polyelectrolytes for application in MEGs with both high voltage and high current outputs. Moreover, we demonstrated the universality of this bilayer sandwich nanocellulose-salt engineering strategy with other anions and cations, exhibiting similar power generation ability, indicating that it could be the next generation of sustainable MEGs with low cost, easier operation, and high performance.

Theoretical Determination of the Electronic Structures and Energy-Level Splitting for Pr3+-Doped Y2SiO5 Crystals.

Trivalent praseodymium (Pr3+)-doped yttrium silicate (Y2SiO5) crystals have been widely used in various phosphors owing to their excellent luminescence characteristics. Although a series of studies have been carried out on its application prospects, the electronic structures and energy-transfer mechanisms of Pr3+-doped Y2SiO5 (Y2SiO5:Pr) remain an exploratory topic. Herein, the crystal structure analysis by the particle swarm optimization structure search method is used to study the structural evolution of Y2SiO5:Pr. Two novel structures with local [PrO7]-11 and [PrO6]-9 [Y2SiO5:Pr (I) and Y2SiO5:Pr (II)] are successfully identified. The impurity Pr3+ ions occupy the Y3+ sites and successfully integrate into the Y2SiO5 host crystal with a Pr3+ concentration of 6.25%. The calculated electronic band structures show that the doping of Pr3+ induces a reduction in band gaps for the host Y2SiO5 crystal. The conduction bands near the Fermi level are completely composed of f states. For the atomic energies of Pr3+ in Y2SiO5, the Stark levels and transitions are properly simulated based on a new set of crystal field parameters (CFPs) at the C1 site symmetry. A satisfactory r.m.s. dev. of 15.57 cm-1 with 9 free ion parameters (plus 27 fixed CFPs as obtained from ab initio calculation) fitted to the 33 observed levels is obtained for the first time. The plentiful energy-level transition lines, from the visible light to the near-infrared region, are deciphered for Pr3+ in Y2SiO5. Blue 3P0 → 3H4 at 465 nm is calculated to be a strong emission line, and it might be an ideal channel for laser actions. These results could not only provide important insights into the rare-earth-doped crystals but also lay the foundation for future research studies of designing the new laser materials.

Three years follow-up of neoadjuvant chemoimmunotherapy in resectable non-small cell lung cancer.

Neoadjuvant chemoimmunotherapy plays a crucial role in resectable non-small cell lung cancer (NSCLC). Neoadjuvant chemotherapy before sleeve lobectomy was safe and feasible, but the impact of neoadjuvant chemoimmunotherapy before sleeve lobectomy was unclear. In our retrospective study, patients diagnosed as stage IIB to IIIB resectable NSCLC between December 1, 2018 and December 1, 2020 in the Department of Thoracic Surgery, Zhejiang Cancer Hospital were collected. We analyzed the efficacy and safety of neoadjuvant chemoimmunotherapy for resectable NSCLC patients and analyzed the impact of different types of surgery on postoperative complications, surgical difficulty, and long-term survival. In total, 56 patients were included in this retrospective study. With a median follow-up of 35 months, 1-year EFS, 2-year EFS, and 3-year EFS were 87.5%, 80.4%, and 76.7%, respectively. 1-year OS, 2-year OS, and 3-year OS were 96.4%, 91.1%, and 85.6%. respectively. Both median EFS and OS were not reached. The percentage of patients with pCR was 51.8%. 48 (85.7%) patients had nodal downstaging and primary tumor downstaging. In 40 (61.4%) patients occurred neoadjuvant chemoimmunotherapy-related adverse events (AEs), most of them of Grade 1 and 2. Postoperative complications occurred in 19 (33.9%) patients. Subgroup analysis showed that sleeve lobectomy was related to better survival and had no impact on operation duration, hospital stay, intraoperative blood loss, and postoperative complications. Neoadjuvant chemoimmunotherapy led to a high pCR rate, favorable 3-year survival rate, and acceptable AEs. Sleeve lobectomy was safe and related to better survival.

Photoluminescence and energy transfer mechanisms of Tm3+ doped Y2O3 laser crystals: experimental and theoretical insights.

Rare-earth thulium (Tm3+) doped yttrium oxide (Y2O3) host single crystals are promising "eye-safe" laser materials. However, the mechanisms of photoluminescence and energy transfer in Tm3+ doped Y2O3 crystals are not yet understood at the fundamental level. Here, we synthetize a series of Y2O3:Tm3+ samples by the sol-gel method. Our experimental results show that the most intensive absorption line of the 3H6 → 1D2 transition occurs at 358 nm, and the strongest emission line of the 1D2 → 3F4 transition is located at 453 nm, which are in good agreement with the calculations of 363 nm and 458 nm, respectively. By using the CALYPSO structural search method, the ground state structure of Y2O3:Tm3+ with P2 space group symmetry is uncovered. The complete energy levels, including free-ion LS terms and crystal-field LSJ multiplet manifolds, of Y2O3:Tm3+ are obtained based on our developed WEPMD method. The present findings show that our WEPMD method can be used in experiments to elucidate the underlying mechanisms of photoluminescence and energy transfer in Tm3+ doped Y2O3 crystals, which offer insights for further understanding of other rare-earth doped laser materials.

Durability Performance Investigation for Engineering Fiber Cementitious Composites (ECC): Review.

Engineered Cementitious Composite (ECC) is currently receiving more and more attention due to its excellent tensile strain hardening and multiple cracking properties. However, due to the high material cost of polyvinyl alcohol (PVA) fiber and quartz sand, its widespread promotion and application in the market are limited. Therefore, scholars at home and abroad have conducted many active studies on improving ECC. This paper summarizes the development history and research status of ECC materials, summarizes the current domestic and foreign researchers' improvement methods for ECC materials, and classifies the improvement methods into three categories: the type of fiber variation, the water-binder ratio variation and adding mineral admixtures, the influences of the above three factors on the mechanical properties and durability of ECC, such as compressive and flexural resistance, are described in detail, and the mechanism of action is explained. Furthermore, this paper introduces the most common uniaxial compression and uniaxial tension constitutive models of ECC. They are briefly classified and evaluated, hoping to help readers' numerical simulation analysis. Finally, some suggestions for ECC research, such as the proportion of water binders and the application of composite fibers, require further research.

Road Performance Investigation on Fiber-Reinforced Recycled Cement Base Material.

The characteristics of the materials used in early buildings in China have led to a large proportion of discarded red bricks among the construction waste generated by demolishing abandoned buildings. The application of red brick aggregate with a particle size ≤5 mm and red brick powder with particle size 0.125~0.75 mm (referred to as recycled brick powder) was studied in this study after the crushing of waste red brick in road structures. The research results will provide a theoretical basis for the whole-grain recycling of waste red brick aggregate. The aggregate of red brick with a particle size smaller than 2 mm was mixed with different amounts of cement soil and fiber to prepare a cement-stable binder for the sub-base material. The recycled brick powder of 0.125~0.75 mm was used to replace the quartz sand with different substitution rates. As pavement materials, different amounts of fiber were used to prepare fiber-reinforced recycled-brick-powder cementitious composites. The optimal mixing ratio of the two materials was evaluated from the mechanical properties. The results showed that the optimal mixing ratio of the cement-stable binder was as follows: waste-red-brick-aggregate content was 50%, cement content was 4%, and fiber content was 0.2%. The optimum ratio of fiber-reinforced recycled-brick-powder cementitious composites was determined to be as follows: the replacement rate of recycled brick powder is 25%, and the content of PVA fiber is 1%. The regression analysis was used to fit the equations between the fiber content and the 7d unconfined compressive strength and the tensile strength of the cement-stabilized binder for different red-brick-aggregate admixtures at 4% cement content. A scanning electron microscope was used to observe the failure modes of the fiber. The influence of failure modes, such as pulling out, fracture, and plastic deformation, on the mechanical properties was expounded.

Performance of Building Solid Waste Powder in Cement Cementitious Material: A Review.

Recycled powder (RP) is a by-product of preparing recycled aggregates from construction waste through debris removal, step-by-step crushing, screening, and mechanical strengthening. It is a fine powder with a particle size of less than 75 µm. Reasonable use of RP can increase the utilization rate of construction waste and reduce dust pollution. This study introduces the current research status of RP. It describes the source of RP; the activation mode of activity; the effect on several aspects, such as early performance and mechanical properties of cement-based materials; and its mechanism of action in light of the research and development. Moreover, the linear regression analysis method was used to obtain the mathematical model between the content of RP and the performance of cement-based materials. The correlation degree between the content of RP and the performance of cement-based materials was obtained based on the gray relation analysis method. It was concluded that the change of the content of RP had the most significant influence on the compressive strength of foamed concrete over 28 d. Finally, some feasible suggestions and prospects for RP are provided.

Efficacy of Concurrent Chemoradiotherapy With S-1 vs Radiotherapy Alone for Older Patients With Esophageal Cancer: A Multicenter Randomized Phase 3 Clinical Trial.

IMPORTANCE: Most older patients with esophageal cancer cannot complete the standard concurrent chemoradiotherapy (CCRT). An effective and tolerable chemoradiotherapy regimen for older patients is needed. OBJECTIVE: To evaluate the efficacy and toxic effects of CCRT with S-1 vs radiotherapy (RT) alone in older patients with esophageal cancer. DESIGN, SETTING, AND PARTICIPANTS: A randomized, open-label, phase 3 clinical trial was conducted at 23 Chinese centers between June 1, 2016, and August 31, 2018. The study enrolled 298 patients aged 70 to 85 years. Eligible participants had histologically confirmed esophageal cancer, stage IB to IVB disease based on the 6th edition of the American Joint Committee on Cancer (stage IVB: only metastasis to the supraclavicular/celiac lymph nodes) and an Eastern Cooperative Oncology Group performance status of 0 to 1. Data analysis was performed from August 1, 2020, to March 10, 2021. INTERVENTIONS: Patients were stratified according to age (<80 vs ≥80 years) and tumor length (<5 vs ≥5 cm) and randomly assigned (1:1) to receive either CCRT with S-1 or RT alone. MAIN OUTCOMES AND MEASURES: The primary end point was the 2-year overall survival rate using intention-to-treat analysis. RESULTS: Of the 298 patients enrolled, 180 (60.4%) were men. The median age was 77 (interquartile range, 74-79) years in the CCRT group and 77 (interquartile range, 74-80) years in the RT alone group. A total of 151 patients (50.7%) had stage III or IV disease. The CCRT group had a significantly higher complete response rate than the RT group (41.6% vs 26.8%; P = .007). Surviving patients had a median follow-up of 33.9 months (interquartile range: 28.5-38.2 months), and the CCRT group had a significantly higher 2-year overall survival rate (53.2% vs 35.8%; hazard ratio, 0.63; 95% CI, 0.47-0.85; P = .002). There were no significant differences in the incidence of grade 3 or higher toxic effects between the CCRT and RT groups except that grade 3 or higher leukopenia occurred in more patients in the CCRT group (9.5% vs 2.7%; P = .01). Treatment-related deaths were observed in 3 patients (2.0%) in the CCRT group and 4 patients (2.7%) in the RT group. CONCLUSIONS AND RELEVANCE: In this phase 3 randomized clinical trial, CCRT with S-1 was tolerable and provided significant benefits over RT alone in older patients with esophageal cancer. TRIAL REGISTRATION: ClinicalTrials.gov Identifier: NCT02813967.

Influence of body mass index on the long-term outcomes of patients with esophageal squamous cell carcinoma who underwent esophagectomy as a primary treatment: A 10-year medical experience.

We explored the influence of body mass index (BMI) on long-term outcomes in patients with esophageal squamous cell carcinoma (ESCC) who underwent esophagectomy as a primary treatment. BMI is a risk factor for development of esophageal cancer. However, the details of the relationship between BMI and cancer prognosis remains unclear. Patients who underwent esophagectomy as an initial treatment in 2000 to 2009 period were included. The patients were divided into 3 groups according to Asian-specific BMI cut-offs. The associations between BMI and long-term outcomes were explored. This study included 1082 ESCC patients between 2000 and 2009; all the patients underwent esophagectomy. The median overall survival (OS) of the BMI <18.5, 18.5 ≤ BMI <23, and BMI ≥23 kg/m groups were 21, 24, and 29.5 months, respectively; they differed significantly (P = 0.005). The 5-year survival rates of the 3 groups were 24.6%, 30.4%, and 35.3%, respectively. Multivariate analysis showed that lower BMI was an independent risk factor for a shorter OS (18.5 ≤ BMI <23 kg/m vs. BMI ≥23 kg/m, hazard ratio [HR] = 1.18; 95% confidence interval [CI] = 1.00-1.40, P = 0.054, BMI <18.5 kg/m vs. BMI ≥23 kg/m, HR = 1.38; 95% CI = 1.09-1.75, P = 0.007). The better OS of the BMI ≥23 kg/m patients remained statistically significant in never-smoking patients (P < 0.05). In conclusion, patients with BMIs ≥23 kg/m experienced better OS, and multivariate analysis further indicated that BMI ≥23 kg/m was an independent predictor of survival. When stratified by smoking status, BMI ≥23 kg/m was still a factor in better OS among never smokers.

Construction of the isocopalane skeleton: application of a desulfinylative 1,7-hydrogen atom transfer strategy.

Two attractive chirons, aldehyde 6 and chloride 7, exhibiting functionalized ent-spongiane-type tricyclic skeletons (ABC ring system), have been constructed and their absolute configurations have been studied by NMR spectroscopy and confirmed by single-crystal X-ray diffraction. Both of these chirons are derived from commercially available andrographolide in good yield. Aldehyde 6 is obtained through a novel K2 S2 O8 -catalyzed aquatic ring-closing reaction of allylic sodium sulfonate and intramolecular 1,7-hydrogen atom transfer process. Further mechanistic investigations demonstrate that the 1,7-hydrogen atom transfer is a free-radical process, whereby hydrogen migrates from C18 to C17, as evidenced by double-18- deuterium-labeled isotope experiments. Prospective applications of these two chiral sources are also discussed.

Elevated levels of preoperative circulating CD44⁺ lymphocytes and neutrophils predict poor survival for non-small cell lung cancer patients.

BACKGROUND: Certain circulating cells have been shown to predict the clinical outcome of several cancers. The objective of this study was to identify clinical, hematological and immunological predictors of prognosis in non-small cell lung cancer (NSCLC) patients. METHODS: A retrospective study on a prevalent cohort of 225 NSCLC patients hospitalized at the Zhejiang Province Cancer Hospital (ZPCH) was conducted from August 1, 2006 to April 15, 2008. Circulating lymphocytes were measured by flow cytometry. WBC count and classification in peripheral blood were measured with a Coulter counter. We calculated the proportion of patients surviving after first hospital admission and hazard ratios (HR) using the Cox proportional hazards model. RESULTS: Elevated levels of preoperative circulating CD44(+) lymphocytes, WBCs and neutrophils indicated low cumulative survival. Clinical stage (HR: 2.292; 95% confidence interval (CI): 1.34-3.91, P=0.002), neutrophils (HR: 1.877; 95% CI: 1.34-2.62, P<0.001) and CD44(+) lymphocytes (HR: 1.018; 95% CI: 1.00-1.03, P=0.002) are independent predictors of survival in NSCLC patients, respectively. Elevated levels of CD44(+) lymphocytes and neutrophils correlated with distant metastasis and prognosis in NSCLC patients with stage III/IV, respectively. CONCLUSIONS: CD44(+) lymphocytes along with neutrophils could serve as an independent prognostic marker for NSCLC patients.

Apoptosis induction of ZBB-006, a novel synthetic diterpenoid, in the human hepatocellular carcinoma cell line HepG2 in vitro and in vivo.

Diterpenes, present in many medicinal plants, have been the focus of continuous studies for the development of new anticancer agents. ZBB-006 is a new synthetic diterpenoid derivative which exhibited significant anti-proliferation activity against various cancer cell lines in our previous study. Here, we investigated the antitumor effect of ZBB-006 and its potential mechanisms in the human hepatocellular carcinoma cell line HepG2, both in vitro and in vivo. We found that oral administration of ZBB-006 effectively suppressed the growth of HepG2 xenograft tumor in nude mice without body weight decline as compared with the control group. Meanwhile, the growth inhibitory effect of ZBB-006 on HepG2 cells was observed with MTT assay. Apoptosis induced by ZBB-006 in HepG2 cells was evidenced by DAPI staining and Annexin V/PI double staining assay. ZBB-006 also dissipated the mitochondrial membrane potential (ΔΨm) apparently as revealed by JC-1 staining. Furthermore, the cleavage of PARP, activation of caspase-3 and caspase-9 but not caspase-8 was demonstrated by western blot assay both in vitro and in vivo. Additionally, the proapoptotic protein Bax was markedly elevated, while the antiapoptotic protein Bcl-2 was downregulated. Collectively, our data indicated that ZBB-006 exerted a strong antitumor effect on HepG2 cells by initiating the mitochondrial-dependent apoptosis, and it has potential to be explored as a new promising therapeutic agent against human hepatoma.