Nanostructured Fe-N-C materials represent a new type of "platinum-like" non-noble-metal catalyst for various electrochemical reactions and organic transformations. However, no consensus has been reached on the active sites of the Fe-N-C catalysts because of their heterogeneity in particle size and composition. In this contribution, we have successfully prepared atomically dispersed Fe-N-C catalyst, which exhibited high activity and excellent reusability for the selective oxidation of the C-H bond. A wide scope of substrates, including aromatic, heterocyclic, and aliphatic alkanes, were smoothly oxidized at room temperature, and the selectivity of corresponding products reached as high as 99%. By using sub-ångström-resolution HAADF-STEM in combination with XPS, XAS, ESR, and Mössbauer spectroscopy, we have provided solid evidence that Fe is exclusively dispersed as single atoms via forming FeN (x = 4-6) and that the relative concentration of each FeN species is critically dependent on the pyrolysis temperature. Among them, the medium-spin FeN affords the highest turnover frequency (6455 h), which is at least 1 order of magnitude more active than the high-spin and low-spin FeN structures and 3 times more active than the FeN structure, although its relative concentration in the catalysts is much lower than that of the FeN structures.
<b><i>Background:</i></b> Primary liver cancer, around 90% are hepatocellular carcinoma in China, is the fourth most common malignancy and the second leading cause of tumor-related death, thereby posing a significant threat to the life and health of the Chinese people. <b><i>Summary:</i></b> Since the publication of <i>Guidelines for Diagnosis and Treatment of Primary Liver Cancer (2017 Edition)</i> in 2018, additional high-quality evidence has emerged with relevance to the diagnosis, staging, and treatment of liver cancer in and outside China that requires the guidelines to be updated. The new edition <i>(2019 Edition)</i> was written by more than 70 experts in the field of liver cancer in China. They reflect the real-world situation in China regarding diagnosing and treating liver cancer in recent years. <b><i>Key Messages:</i></b> Most importantly, the new guidelines were endorsed and promulgated by the Bureau of Medical Administration of the National Health Commission of the People’s Republic of China in December 2019.
The single-atom Co–N–C catalyst with the structure of CoN4C8-1-2O2 shows excellent performance for the chemoselective hydrogenation of nitroarenes to produce azo compounds under mild reaction conditions.
<b><i>Background:</i></b> Radiomics has emerged as a new approach that can help identify imaging information associated with tumor pathophysiology. We developed and validated a radiomics nomogram for preoperative prediction of microvascular invasion (MVI) in hepatocellular carcinoma (HCC). <b><i>Methods:</i></b> Two hundred and eight patients with pathologically confirmed HCC (training cohort: <i>n</i> = 146; validation cohort: <i>n</i> = 62) who underwent preoperative gadoxetic acid-enhanced magnetic resonance (MR) imaging were included. Least absolute shrinkage and selection operator logistic regression was applied to select features and construct signatures derived from MR images. Univariate and multivariate analyses were used to identify the significant clinicoradiological variables and radiomics signatures associated with MVI, which were then incorporated into the predictive nomogram. The performance of the radiomics nomogram was evaluated by its calibration, discrimination, and clinical utility. <b><i>Results:</i></b> Higher α-fetoprotein level (<i>p</i> = 0.046), nonsmooth tumor margin (<i>p</i> = 0.003), arterial peritumoral enhancement (<i>p <</i> 0.001), and the radiomics signatures of hepatobiliary phase (HBP) T1-weighted images (<i>p <</i> 0.001) and HBP T1 maps (<i>p <</i> 0.001) were independent risk factors of MVI. The predictive model that incorporated the clinicoradiological factors and the radiomic features derived from HBP images outperformed the combination of clinicoradiological factors in the training cohort (area under the curves [AUCs] 0.943 vs. 0.850; <i>p</i> = 0.002), though the validation did not have a statistical significance (AUCs 0.861 vs. 0.759; <i>p</i> = 0.111). The nomogram based on the model exhibited C-index of 0.936 (95% CI 0.895–0.976) and 0.864 (95% CI 0.761–0.967) in the training and validation cohort, fitting well in calibration curves (<i>p</i> > 0.05). Decision curve analysis further confirmed the clinical usefulness of the nomogram. <b><i>Conclusions:</i></b> The nomogram incorporating clinicoradiological risk factors and radiomic features derived from HBP images achieved satisfactory preoperative prediction of the individualized risk of MVI in patients with HCC.
Black carbon (BC) emissions from China are of global concern. A new BC emission inventory (PKU-BC(China)) has been developed with the following improvements: (1) The emission factor database was updated; (2) a 0.1° × 0.1° gridded map was produced for 2007 based on county-level proxies; (3) time trends were derived for 1949-2007 and predicted for 2008-2050; and (4) the uncertainties associated with the inventory were quantified. It was estimated that 1957 Gg of BC were emitted in China in 2007, which is greater than previously reported. Residential coal combustion was the largest source, followed by residential biofuel burning, coke production, diesel vehicles, and brick kilns. By using a county-level disaggregation method, spatial bias in province-level disaggregation, mainly due to uneven per capita emissions within provinces, was reduced by 42.5%. Emissions increased steadily since 1949 until leveling off in the mid-1990s, due to a series of technological advances and to socioeconomic progress. BC emissions in China in 2050 are predicted to be 920-2183 Gg/yr under various scenarios; and the industrial and transportation sectors stand to benefit the most from technological improvements.
Atmospheric particulate matter with diameter <2.5 um (PM2.5) was collected at Peking University (PKU) in Beijing, China before, during, and after the 2008 Olympics and analyzed for black carbon (BC), organic carbon (OC), lower molecular weight (MW<300) and MW302 Polycyclic Aromatic Hydrocarbons (PAHs), nitrated PAHs (NPAHs) and oxygenated PAHs (OPAHs). In addition, the direct and indirect acting mutagenicity of the PM2.5 and the potential for DNA damage to human lung cells were also measured. Significant reductions in BC (45%), OC (31%), MW< 300 PAH (26% – 73%), MW 302 PAH (22% – 77%), NPAH (15% – 68%) and OPAH (25% – 53%) concentrations were measured during the source control and Olympic Olympic period. However, the mutagenicity of the PM2.5 was significantly reduced only during the Olympic period. The PAH, NPAH, and OPAH composition of the PM2.5 was similar throughout the study, suggesting similar sources during the different periods. During the source control period, the parent PAH concentrations were correlated with NO, CO, and SO2 concentrations, indicating that these PAHs were associated with both local and regional emissions. However, the NPAH and OPAH concentrations were only correlated with the NO concentrations, indicating that the NPAH and OPAH were primarily associated with local emissions. The relatively high 2-nitrofluoranthene/1-nitropyrene ratio (25 – 46) and 2-nitrofluoranthene/2-nitropyrene ratio (3.4 – 4.8), suggested a predominance of photochemical formation of NPAHs through OH-radical-initiated reactions in the atmosphere. On average, the ΣNPAH and ΣOPAH concentrations were 8% of the parent PAH concentrations, while the direct-acting mutagenicity (due to the NPAH and OPAH) was 200% higher than the indirect-acting mutagenicity (due to the PAH). This suggests that NPAH and OPAH make up a significant portion of the overall mutagenicity of PM2.5 in Beijing.
Ion exchange resin supported Au alloyed Pd single atoms have been explored to serve as an effective and robust catalyst for the Ullmann reaction of aryl halides under mild conditions in aqueous media, in particular for the activation of less reactive aryl chlorides. The catalysts were prepared with an ion exchange-NaBH 4 reduction method and submitted to extensive characterizations by HRTEM, XRD, EXAFS, and DRIFTS techniques. XRD patterns demonstrated the formation of Au−Pd alloys. EXAFS and DRIFTS characterization results showed that with an increase of Au/Pd molar ratios, the continuous Pd ensembles on the surface were gradually separated and eventually isolated by Au atoms, confirming that the Au alloyed Pd single-atom catalyst was formed. The catalysts exhibited excellent performance for the Ullmann reaction of aryl chlorides, and the turnover number (TON) increased exponentially with a decrease of the amount of Pd in the catalysts. On the basis of these characterization and catalytic results, the Au alloyed Pd single-atom was proposed as the active site for the reaction. The catalyst exhibited excellent catalytic performance for a broad scope of substrates and could be reused at least 8 times with no change in yield. This Au alloyed Pd single-atom catalyst bridges the gap between homogeneous and heterogeneous catalysis in organic transformations and may open a new vision to develop other efficient single-atom catalysts for green synthesis of fine chemicals.
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