Direct Arylation of Benzyl Ethers with Organozinc Reagents

A novel C­(sp³)–H bond arylation of benzyl ethers with Knochel-type arylzinc reagents has been developed. This transition-metal-catalyst-free reaction proceeds well under mild conditions in a simple and effective manner and enables the synthesis of a wide range of potentially biologically active benzyl ethers by using highly functionalized organozinc reagents as a carbon nucleophile

Data-related challenges and solutions in building China’s national carbon emissions trading scheme

<p>China is now in the process of building its national carbon emissions trading scheme (ETS). Data are the foundation for the design and operation of an ETS. This paper presents a comparative analysis of the data requirements for China’s national ETS construction and the existing ETS-related data for enterprises in China. In doing so, it identifies the underlying data gap in building China’s national ETS in terms of data availability and data quality. Based on the experiences of international ETSs, and experiences at national and pilot levels in China, we propose two short-term strategies and four long-term solutions to meet the challenges from technical and management perspectives.</p> <p><b>Key policy insights</b></p><p>The major data requirements for China’s national ETS can be categorized into six groups: production, emissions, technology, management, economy and policy data.</p><p>The ETS-related data are generally available in China except for parts of data on emissions, such as energy carbon content and the oxidation factor.</p><p>The data challenges that are faced by China’s national ETS include differences in corporate data availability and imperfect data quality.</p><p>Short-term strategies to address the challenges include establishing data collection guidelines based on existing data and prioritizing major emissions or sectors with better data for inclusion under the ETS.</p><p>Long-term solutions to address the challenges include introducing the concept of tiers, clarifying data sources and introducing a monitoring plan, conducting MRV capacity building and establishing a rigorous third-party verification system.</p><p></p> <p>The major data requirements for China’s national ETS can be categorized into six groups: production, emissions, technology, management, economy and policy data.</p> <p>The ETS-related data are generally available in China except for parts of data on emissions, such as energy carbon content and the oxidation factor.</p> <p>The data challenges that are faced by China’s national ETS include differences in corporate data availability and imperfect data quality.</p> <p>Short-term strategies to address the challenges include establishing data collection guidelines based on existing data and prioritizing major emissions or sectors with better data for inclusion under the ETS.</p> <p>Long-term solutions to address the challenges include introducing the concept of tiers, clarifying data sources and introducing a monitoring plan, conducting MRV capacity building and establishing a rigorous third-party verification system.</p

Charge Transfer Effects on Resonance-Enhanced Raman Scattering for Molecules Adsorbed on Single-Crystalline Perovskite

Single-crystalline hybrid perovskites have important photoelectronic properties for advanced semiconductor devices, such as solar cells and photodetectors. However, neither the surface-enhanced Raman scattering (SERS) property nor the correlation between SERS and photoelectronic properties for single-crystalline perovskites have ever been studied. Here, for the first time, we observed a 10⁵ enhancement in SERS for 4-mercaptopyridine (MPY) adsorbed on a methylamine lead chlorine (MAPbCl₃) single crystal. Compared to the Raman spectrum of bulk MPY molecules, the b₂ mode of the MPY molecule was selectively enhanced. This is attributed to the charge transfer (CT) resonance mechanism at the interface between the single crystal and the adsorbed molecules, which benefit from the Herzberg–Teller contribution. UV–vis spectra demonstrated that the modification with the MPY molecules leads to the formation of a new interfacial transition state, which matches the excitation laser photon energy and results in a CT resonance process under 532 nm laser excitation. The MPY-modified MAPbCl₃ single crystal was further applied to a photoelectronic device, and the device <i>I–V</i> curve was collected under 532 nm laser irradiation. The results indicate that the MPY-modified MAPbCl₃ shows a clear photoelectronic response to the 532 nm light. This study establishes a correlation between the CT resonance-enhanced Raman and the photoelectronic responses of perovskite materials and provides guidance for future molecule-sensitized perovskite photoelectronic device studies

Charge Transfer Effects on Resonance-Enhanced Raman Scattering for Molecules Adsorbed on Single-Crystalline Perovskite

Single-crystalline hybrid perovskites have important photoelectronic properties for advanced semiconductor devices, such as solar cells and photodetectors. However, neither the surface-enhanced Raman scattering (SERS) property nor the correlation between SERS and photoelectronic properties for single-crystalline perovskites have ever been studied. Here, for the first time, we observed a 10⁵ enhancement in SERS for 4-mercaptopyridine (MPY) adsorbed on a methylamine lead chlorine (MAPbCl₃) single crystal. Compared to the Raman spectrum of bulk MPY molecules, the b₂ mode of the MPY molecule was selectively enhanced. This is attributed to the charge transfer (CT) resonance mechanism at the interface between the single crystal and the adsorbed molecules, which benefit from the Herzberg–Teller contribution. UV–vis spectra demonstrated that the modification with the MPY molecules leads to the formation of a new interfacial transition state, which matches the excitation laser photon energy and results in a CT resonance process under 532 nm laser excitation. The MPY-modified MAPbCl₃ single crystal was further applied to a photoelectronic device, and the device <i>I–V</i> curve was collected under 532 nm laser irradiation. The results indicate that the MPY-modified MAPbCl₃ shows a clear photoelectronic response to the 532 nm light. This study establishes a correlation between the CT resonance-enhanced Raman and the photoelectronic responses of perovskite materials and provides guidance for future molecule-sensitized perovskite photoelectronic device studies

Preparation of a Superhydrophobic and Peroxidase-like Activity Array Chip for H₂O₂ Sensing by Surface-Enhanced Raman Scattering

In this paper, we propose a novel and simple method for preparing a dual-biomimetic functional array possessing both superhydrophobic and peroxidase-like activity that can be used for hydrogen peroxide (H₂O₂) sensing. The proposed method is an integration innovation that combines the above two properties and surface-enhanced Raman scattering (SERS). We integrated a series of well-ordered arrays of Au points (<i>d</i> = 1 mm) onto a superhydrophobic copper (Cu)/silver (Ag) surface by replicating an arrayed molybdenum template. Instead of using photoresists and the traditional lithography method, we utilized a chemical etching method (a substitution reaction between Cu and HAuCl₄) with a Cu/Ag superhydrophobic surface as the barrier layer, which has the benefit of water repellency. The as-prepared Au points were observed to possess peroxidase-like activity, allowing for catalytic oxidation of the chromogenic molecule <i>o</i>-phenylenediamine dihydrochloride (OPD). Oxidation was evidenced by a color change in the presence of H₂O₂, which allows the array chip to act as an H₂O₂ sensor. In this study, the water repellency of the superhydrophobic surface was used to fabricate the array chip and increase the local reactant concentration during the catalytic reaction. As a result, the catalytic reaction occurred when only 2 μL of an aqueous sample (OPD/H₂O₂) was placed onto the Au point, and the enzymatic product, 2,3-diaminophenazine, showed a SERS signal distinguishable from that of OPD after mixing with 2 μL of colloidal Au. Using the dual-biomimetic functional array chip, quantitative analysis of H₂O₂ was performed by observing the change in the SERS spectra, which showed a concentration-dependent behavior for H₂O₂. This method allows for the detection of H₂O₂ at concentrations as low as 3 pmol per 2 μL of sample, which is a considerable advantage in H₂O₂ analysis. The as-prepared substrate was convenient for H₂O₂ detection because only a small amount of sample was required in each analysis. Highly sensitive detection was realized using SERS. Therefore, this chip was shown to exhibit significant potential for applications in bioanalysis

Charge Transfer Effects on Resonance-Enhanced Raman Scattering for Molecules Adsorbed on Single-Crystalline Perovskite

Single-crystalline hybrid perovskites have important photoelectronic properties for advanced semiconductor devices, such as solar cells and photodetectors. However, neither the surface-enhanced Raman scattering (SERS) property nor the correlation between SERS and photoelectronic properties for single-crystalline perovskites have ever been studied. Here, for the first time, we observed a 10⁵ enhancement in SERS for 4-mercaptopyridine (MPY) adsorbed on a methylamine lead chlorine (MAPbCl₃) single crystal. Compared to the Raman spectrum of bulk MPY molecules, the b₂ mode of the MPY molecule was selectively enhanced. This is attributed to the charge transfer (CT) resonance mechanism at the interface between the single crystal and the adsorbed molecules, which benefit from the Herzberg–Teller contribution. UV–vis spectra demonstrated that the modification with the MPY molecules leads to the formation of a new interfacial transition state, which matches the excitation laser photon energy and results in a CT resonance process under 532 nm laser excitation. The MPY-modified MAPbCl₃ single crystal was further applied to a photoelectronic device, and the device <i>I–V</i> curve was collected under 532 nm laser irradiation. The results indicate that the MPY-modified MAPbCl₃ shows a clear photoelectronic response to the 532 nm light. This study establishes a correlation between the CT resonance-enhanced Raman and the photoelectronic responses of perovskite materials and provides guidance for future molecule-sensitized perovskite photoelectronic device studies

Charge Transfer Effects on Resonance-Enhanced Raman Scattering for Molecules Adsorbed on Single-Crystalline Perovskite

Single-crystalline hybrid perovskites have important photoelectronic properties for advanced semiconductor devices, such as solar cells and photodetectors. However, neither the surface-enhanced Raman scattering (SERS) property nor the correlation between SERS and photoelectronic properties for single-crystalline perovskites have ever been studied. Here, for the first time, we observed a 10⁵ enhancement in SERS for 4-mercaptopyridine (MPY) adsorbed on a methylamine lead chlorine (MAPbCl₃) single crystal. Compared to the Raman spectrum of bulk MPY molecules, the b₂ mode of the MPY molecule was selectively enhanced. This is attributed to the charge transfer (CT) resonance mechanism at the interface between the single crystal and the adsorbed molecules, which benefit from the Herzberg–Teller contribution. UV–vis spectra demonstrated that the modification with the MPY molecules leads to the formation of a new interfacial transition state, which matches the excitation laser photon energy and results in a CT resonance process under 532 nm laser excitation. The MPY-modified MAPbCl₃ single crystal was further applied to a photoelectronic device, and the device <i>I–V</i> curve was collected under 532 nm laser irradiation. The results indicate that the MPY-modified MAPbCl₃ shows a clear photoelectronic response to the 532 nm light. This study establishes a correlation between the CT resonance-enhanced Raman and the photoelectronic responses of perovskite materials and provides guidance for future molecule-sensitized perovskite photoelectronic device studies

Charge-Transfer Effect on Surface-Enhanced Raman Scattering (SERS) in an Ordered Ag NPs/4-Mercaptobenzoic Acid/TiO₂ System

With the explosive development of analysis and detection techniques based on surface-enhanced Raman scattering (SERS), the further understanding and exploitation of the chemical mechanism becomes particularly important. We investigated the charge transfer (CT) effect on SERS in a semiconductor–molecule–metal system constructed with Ag NPs, 4-mercaptobenzoic acid (MBA) molecule, and atomic level TiO₂. To ensure more ordering, the system is constructed by a layer-by-layer self-assembly method. After introducing TiO₂, we found that the relative band intensity of some peaks displayed a distinct difference, which is attributed to the Herzberg–Teller contribution that occurs via CT. We also proposed a possible mechanism responsible for the selective enhancement observed in the SERS spectra of the Ag NPs/MBA/TiO₂ system. This work will not only provide much deeper insight into the CT mechanism in SERS but also help in the development of a method to construct metal–semiconductor-based SERS substrates

Additional file 5: of Association between inflammation and systolic blood pressure in RA compared to patients without RA

Table S1. Association between change in C-reactive protein (CRP) (per 10 mg/L) and change in diastolic blood pressure (DBP), pulse pressure (PP), and mean arterial pressure (MAP) (per mmHg) in patients with rheumatoid arthritis with significant changes in inflammation. (DOCX 17 kb

Additional file 4: of Association between inflammation and systolic blood pressure in RA compared to patients without RA

Figure S4. The relationship between C-reactive protein levels (CRP) and systolic blood pressure with 95% confidence intervals, in the non-RA outpatient population and general population (NHANES) with trimming of extreme measurements of CRP (< 0.5% and > 99.5%). Non-RA outpatient population CRP range 0.10–142.20 mg/L; NHANES CRP range 0.02–4.22 mg/L. RA, rheumatoid arthritis; NHANES, National Health and Nutrition Examination Survey. (PDF 471 kb