Surface Redox Chemistry Regulates the Reaction Microenvironment for Efficient Hydrogen Peroxide Generation.

Electrosynthesis has emerged as an enticing solution for hydrogen peroxide (H2O2) production. However, efficient H2O2 generation encounters challenges related to the robust gas-liquid-solid interface within electrochemical reactors. In this work, we introduce an effective hydrophobic coating modified by iron (Fe) sites to optimize the reaction microenvironment. This modification aims to mitigate radical corrosion through Fe(II)/Fe(III) redox chemistry, reinforcing the reaction microenvironment at the three-phase interface. Consequently, we achieved a remarkable yield of up to 336.1 mmol h-1 with sustained catalyst operation for an extensive duration of 230 h at 200 mA cm-2 without causing damage to the reaction interface. Additionally, the Faradaic efficiency of H2O2 exceeded 90% across a broad range of test current densities. This surface redox chemistry approach for manipulating the reaction microenvironment not only advances long-term H2O2 electrosynthesis but also holds promise for other gas-starvation electrochemical reactions.

Mechanofluorochromic behaviors and data security protection properties of salicylaldimine-based difluoroboron complexes with different aryl substituents.

To further explore the relationship between aryl substituents and mechanofluorochromic (MFC) behaviors, four salicylaldimine-based difluoroboron complexes (ts-Ph BF2, ts-Ph-NA BF2, ts-2NA BF2, and ts-triphenylamine [TPA] BF2), including aromatic substituents with different steric hindrance effects, were designed and successfully synthesized. Four complexes with twisted molecular conformation displayed intramolecular charge transfer and aggregation-induced emission properties. Under external mechanical stimuli, the as-synthesized powders of ts-Ph BF2, ts-Ph-NA BF2, and ts-TPA BF2 exhibited redshift fluorescence emission behaviors, and ts-Ph BF2 and ts-TPA BF2 could be recovered to original shifts by fuming, but ts-Ph-NA BF2 displayed irreversible switching. ts-2NA BF2 had no change during the grinding and fuming processes. The results indicated that the MFC behaviors could be attributed to the phase transformation between the well-defined crystalline and disordered amorphous states by X-ray diffraction measurement. Further research illustrated that ts-TPA BF2 with the most significant MFC phenomenon could be applied in data security protection in ink-free rewritable paper.

RhNi Bimetallenes with Lattice-Compressed Rh Skin towards Ultrastable Acidic Nitrate Electroreduction.

Harvesting recyclable ammonia (NH3 ) from acidic nitrate (NO3 - )-containing wastewater requires the utilization of corrosion-resistant electrocatalytic materials with high activity and selectivity towards acidic electrochemical nitrate reduction (NO3 ER). Herein, ultrathin RhNi bimetallenes with Rh-skin-type structure (RhNi@Rh BMLs) are fabricated towards acidic NO3 ER. The Rh-skin atoms on the surface of RhNi@Rh BMLs experience the lattice compression-induced strain effect, resulting in shortened Rh-Rh bond and downshifted d-band center. Experimental and theoretical calculation results corroborate that Rh-skin atoms can inhibit NO2 */NH2 * adsorption-induced Rh dissolution, contributing to the exceptional electrocatalytic durability of RhNi@Rh BMLs (over 400 h) towards acidic NO3 ER. RhNi@Rh BMLs also reveal an excellent catalytic performance, boasting a 98.4% NH3 Faradaic efficiency and a 13.4 mg h-1 mgcat -1 NH3 yield. Theoretical calculations reveal that compressive stress tunes the electronic structure of Rh skin atoms, which facilitates the reduction of NO* to NOH* in NO3 ER. The practicality of RhNi@Rh BMLs has also been confirmed in an alkaline-acidic hybrid zinc-nitrate battery with a 1.39 V open circuit voltage and a 10.5 mW cm-2 power density. This work offers valuable insights into the nature of electrocatalyst deactivation behavior and guides the development of high-efficiency corrosion-resistant electrocatalysts for applications in energy and environment.

Low-coordination Nanocrystalline Copper-based Catalysts through Theory-guided Electrochemical Restructuring for Selective CO2 Reduction to Ethylene.

Revealing the dynamic reconstruction process and tailoring advanced copper (Cu) catalysts is of paramount significance for promoting the conversion of CO2 into ethylene (C2H4), paving the way for carbon neutralization and facilitating renewable energy storage. In this study, we initially employed density functional theory (DFT) and molecular dynamics (MD) simulations to elucidate the restructuring behavior of a catalyst under electrochemical conditions and delineated its restructuring patterns. Leveraging insights into this restructuring behavior, we devised an efficient, low-coordination copper-based catalyst. The resulting synthesized catalyst demonstrated an impressive Faradaic efficiency (FE) exceeding 70 % for ethylene generation at a current density of 800 mA cm-2. Furthermore, it showed robust stability, maintaining consistent performance for 230 hours at a cell voltage of 3.5 V in a full-cell system. Our research not only deepens the understanding of the active sites involved in designing efficient carbon dioxide reduction reaction (CO2RR) catalysts but also advances CO2 electrolysis technologies for industrial application.

EEGProgress: A fast and lightweight progressive convolution architecture for EEG classification.

Because of the intricate topological structure and connection of the human brain, extracting deep spatial features from electroencephalograph (EEG) signals is a challenging and time-consuming task. The extraction of topological spatial information plays a crucial role in EEG classification, and the architecture of the spatial convolution greatly affects the performance and complexity of convolutional neural network (CNN) based EEG classification models. In this study, a progressive convolution CNN architecture named EEGProgress is proposed, aiming to efficiently extract the topological spatial information of EEG signals from multi-scale levels (electrode, brain region, hemisphere, global) with superior speed. To achieve this, the raw EEG data is permuted using the empirical topological permutation rule, integrating the EEG data with numerous topological properties. Subsequently, the spatial features are extracted by a progressive feature extractor including prior, electrode, region, and hemisphere convolution blocks, progressively extracting the deep spatial features with reduced parameters and speed. Finally, the comparison and ablation experiments under both cross-subject and within-subject scenarios are conducted on a public dataset to verify the performance of the proposed EEGProgress and the effectiveness of the topological permutation. The results demonstrate the superior feature extraction ability of the proposed EEGProgress, with an average increase of 4.02% compared to other CNN-based EEG classification models under both cross-subject and within-subject scenarios. Furthermore, with the obtained average testing time, FLOPs, and parameters, the proposed EEGProgress outperforms other comparison models in terms of model complexity.

Association of ultra-processed foods consumption with risk of cardio-cerebrovascular disease: A systematic review and meta-analysis of cohort studies.

AIMS: The epidemiological evidence regarding the impact of ultra-processed foods (UPFs) on the risk of cardio-cerebrovascular diseases (CCVDs) is controversial. The aim of this systematic review and meta-analysis is to examine the association between UPF consumption and the risk of CCVDs within cohort studies. DATA SYNTHESIS: A systematic literature search was conducted across multiple databases, including PubMed/Medline, Embase, Web of Science, Scopus, and the Cochrane Library databases, covering the inception of these databases up until January 1st, 2023. A total of 39 cohort studies involving 63,573,312 human participants were deemed eligible according to the inclusion criteria. Utilizing random-effects models, risk ratios (RRs) were estimated to determine the pooled results. Our findings indicate a significant association between a higher consumption of UPF and an increased likelihood of CCVDs (RR: 1.08, 95% CI: 1.01-1.16, I2 = 89%; p < 0.01) compared to individuals who either abstain from or consume lesser amounts of UPF. Nonlinear dose-response meta-analyses showed that a consistent high intake of UPFs was associated with an elevated risk of developing CCVDs (p non-linearity <0.001). Notably, the risk of CCVDs escalated by approximately 7% with an UPF intake of up to 1 serving per day. Subgroup analysis further revealed a significant augmentation in the risk of total CVD and hypertension with increased UPF consumption. CONCLUSIONS: A higher intake of UPF significantly increases the risk of developing CCVDs. Prospective studies controlling for confounding factors are needed to validate the relationship between UPF intake and the development of CCVDs.

Regulated Zn Plating and Stripping by a Multifunctional Polymer-Alloy Interphase Layer for Stable Zn Metal Anode.

Metallic zinc electrode with a high theoretical capacity of 820 mAh g-1 is highly considered as a promising candidate for next-generation rechargeable batteries. However, the unavoidable hydrogen evolution, uncontrolled dendrite growth, and severe passivation reaction badly hinder its practical implementations. Herein, a robust polymer-alloy artificial protective layer is designed to realize dendrite-free Zn metal anode by the integration of zincophilic SnSb nanoparticles with Nafion. In comparison to the bare Zn electrode, the Nafion-SnSb coated Zn (NFSS@Zn) electrode exhibits lower nucleation energy barrier, more uniform electric field distribution and stronger anti-corrosion capability, thus availably suppressing the Zn dendrite growth and interfacial side reactions. As a consequence, the NFSS@Zn electrode exhibits a long cycle life over 1500 h at 1 mA cm-2 with an ultra-low voltage hysteresis (25 mV). Meanwhile, when paired with a MnO2 cathode, the as-prepared full cell also demonstrates stable performance for 1000 cycles at 3 A g-1 . This work provides an inspired approach to boost the performance of Zn anodes.

Recent advances in proton exchange membrane water electrolysis.

Proton exchange membrane water electrolyzers (PEMWEs) are an attractive technology for renewable energy conversion and storage. By using green electricity generated from renewable sources like wind or solar, high-purity hydrogen gas can be produced in PEMWE systems, which can be used in fuel cells and other industrial sectors. To date, significant advances have been achieved in improving the efficiency of PEMWEs through the design of stack components; however, challenges remain for their large-scale and long-term application due to high cost and durability issues in acidic conditions. In this review, we examine the latest developments in engineering PEMWE systems and assess the gap that still needs to be filled for their practical applications. We provide a comprehensive summary of the reaction mechanisms, the correlation among structure-composition-performance, manufacturing methods, system design strategies, and operation protocols of advanced PEMWEs. We also highlight the discrepancies between the critical parameters required for practical PEMWEs and those reported in the literature. Finally, we propose the potential solution to bridge the gap and enable the appreciable applications of PEMWEs. This review may provide valuable insights for research communities and industry practitioners working in these fields and facilitate the development of more cost-effective and durable PEMWE systems for a sustainable energy future.

Meet the Editorial Board: an introduction to and insights from Fumin Li.

Jack Lodge, Commissioning Editor of Bioanalysis, and Neil Spooner, Editor-in-Chief, speak to Fumin Li.

Regulating Reversible Oxygen Electrocatalysis by Built-in Electric Field of Heterojunction Electrocatalyst with Modified d-Band.

Developing bifunctional catalysts for oxygen electrochemical reactions is essential for high-performance electrochemical energy devices. Here, a Mott-Schottky heterojunction composed of porous cobalt-nitrogen-carbon (Co-N-C) polyhedra containing abundant metal-phosphides for reversible oxygen electrocatalysis is reported. As a demonstration, this catalyst shows excellent activity in the oxygen electrocatalysis and thus delivers outstanding performance in rechargeable zinc-air batteries (ZABs). The built-in electric field in the Mott-Schottky heterojunction can promote electron transfer in oxygen electrocatalysis. More importantly, an appropriate d-band center of the heterojunction catalyst also endows oxygen intermediates with a balanced adsorption/desorption capability, thus enhancing oxygen electrocatalysis and consequently improving the performance of ZABs. The work demonstrates an important design principle for preparing efficient multifunctional catalysts in energy conversion technologies.

Soil exposure is the major fluoride exposure pathways for residents from the high-fluoride karst region in Southwest China.

In the karst areas of southwest China, soil fluoride levels are higher than in China (478 mg kg-1) and world (200 mg kg-1). High levels of F in the environment might pose a health risk to humans. The comprehensive exposure risk must be studied in this area. Herein, samples of crops and soil were collected from Bijie City, a typical karst area in southwest China, to investigate the pollution level and evaluate the comprehensive F exposure risk. The single-factor index (PFw) and the geological accumulation index (Igeo) were used. The hazard index (HI) was applied to assess exposure risk from multiple exposure routes. The results revealed that there is considerable F contamination in soil and crops in the study area. Average soil total fluorine (Ft) was 1139.13 mg kg-1, and soil water soluble F (Fw) was 3.792 mg kg-1. In corn, rice, wheat, and potatoes, F contents were 1.167-9.585, 1.222-6.698, 1.587-9.976, and 1.797-9.143 mg kg-1, respectively. The mean values of HI were 4.45 and 2.42 for children and adults, respectively, > 1, showing potential health risk exists. Youngsters are at a greater exposure risk than adults. From the results of contribution ratios of different exposure routes for health risk, the major exposure risk was determined to be from soil exposure. Based on this, we suggest that risk managers mainly strive to control the soil fluoride level and implement the risk education and communication.

Classroom compositional effects on low-ability students' achievement in China.

Peer effects are at the center of educational policy debates regarding school choice, ability grouping, and instructional design. Though emerging empirical evidence suggests that positive peer effects exist, less is known about how it affects students with varying cognitive abilities. Using a nationally representative sample from China, we generated a student-level measure of classroom composition of peers based on cognitive ability to understand the benefits or pitfalls of placing low-ability students with heterogeneous or homogenous classmates. We conducted this analysis separately for grades seven and nine students after controlling for student background, family characteristics, and school endogeneity. We reaffirmed the overall positive-but small-peer effects on the performance rankings. Low-ability children scored much lower than their counterparts when they studied in cognitively diverse classrooms. However, this effect negates the overall positive impact of studying with high-ability peers and the pattern is consistent across rural and urban schools.

An integrated platinum-nanocarbon electrocatalyst for efficient oxygen reduction.

Efficient and robust platinum-carbon electrocatalysts are of great significance for the long-term service of high-performance fuel cells. Here, we report a Pt alloy integrated in a cobalt-nitrogen-nanocarbon matrix by a multiscale design principle for efficient oxygen reduction reaction. This Pt integrated catalyst demonstrates an increased mass activity, 11.7 times higher than that of commercial Pt catalyst, and retains a stability of 98.7% after 30,000 potential cycles. Additionally, this integrated catalyst delivers a current density of 1.50 A cm-2 at 0.6 V in the hydrogen-air fuel cell and achieves a power density of 980 mW cm-2. Comprehensive investigations demonstrate that the synergistic contribution of components and structure in the platinum-carbon integrated catalyst is responsible for the high-efficiency ORR in fuel cells.

Layered Pd oxide on PdSn nanowires for boosting direct H2O2 synthesis.

Hydrogen peroxide (H2O2) has the wide range of applications in industry and living life. However, the development of the efficient heterogeneous catalyst in the direct H2O2 synthesis (DHS) from H2 and O2 remains a formidable challenge because of the low H2O2 producibility. Herein, we develop a two-step approach to prepare PdSn nanowire catalysts, which comprises Pd oxide layered on PdSn nanowires (PdL/PdSn-NW). The PdL/PdSn-NW displays superior reactivity in the DHS at zero Celcius, presenting the H2O2 producibility of 528 mol kgcat-1·h-1 and H2O2 selectivity of >95%. A layer of Pd oxide on the PdSn nanowire generates bi-coordinated Pd, leading to the different adsorption behaviors of O2, H2 and H2O2 on the PdL/PdSn-NW. Furthermore, the weak adsorption of H2O2 on the PdL/PdSn-NW contributes to the low activation energy and high H2O2 producibility. This surface engineering approach, depositing metal layer on metal nanowires, provides a new insight in the rational designing of efficient catalyst for DHS.

Tax preference, financing constraints and enterprise investment efficiency-Experience, of China's enterprises investment.

This paper takes the 2014 pilot project of accelerated depreciation of fixed assets as a quasi-natural experiment, and builds a Propensity Score Matching-Difference in Differences (PSM-DID) model based on the data of Chinese listed companies from 2000 to 2019 to test the impact of tax preference on enterprise investment efficiency and its mechanism. The results show that the policy inhibits supported enterprises investment efficiency significantly. Heterogeneity analysis shows that the policy causes greater investment efficiency losses for small and medium-sized enterprises, non-state-owned enterprises and asset-heavy enterprises. The mechanism test found the reason why the policy eased financing constraints but inhibited investment efficiency in short-term. After a variety of robustness tests, the above basic conclusions are still valid. Although the accelerated depreciation policy of fixed assets is conducive to expanding the scale of investment, the incentive effect on investment efficiency is not obvious, and even shows a restraining effect. Given the existence of heterogeneity, the design of the policy should not only distinguish industries, but also pay attention to the differences between different enterprises in the same industry. Strengthening research and development (R&D) innovation and improving the matching mechanism between human capital and fixed investment will help give full play to the incentive effect of this policy. The research in this paper helps to deepen the understanding of the microeconomic effects of tax policy and identify the internal mechanism, which not only enriches the relevant literature, but also provides a reference for the government to better use tax policy to promote the high-quality development of enterprises.

Ultrathin rhodium nanosheet-gold nanowire nanocomposites for alkaline methanol oxidation reaction.

Electrostatically assembled ultrathin rhodium nanosheet-gold nanowire nanocomposites (Rh-Au CNSs) were used as an advanced electrocatalyst for the methanol oxidation reaction, which revealed a mass activity of 355 mA mgRh-1 at 0.607 V potential, much higher than single metal Rh nanosheets (273 mA mgRh-1) and commercial Rh nanoparticles (165 mA mgRh-1).

Corrosion Chemistry of Electrocatalysts.

Electrocatalysts are the core components of many sustainable energy conversion technologies that are considered the most potential solution to the worldwide energy and environmental crises. The reliability of structure and composition pledges that electrocatalysts can achieve predictable and stable performance. However, during the electrochemical reaction, electrocatalysts are influenced directly by the applied potential, the electrolyte, and the adsorption/desorption of reactive species, triggering structural and compositional corrosion, which directly affects the catalytic behaviors of electrocatalysts (performance degradation or enhancement) and invalidates the established structure-activity relationship. Therefore, it is necessary to elucidate the corrosion behavior and mechanism of electrocatalysts to formulate targeted corrosion-resistant strategies or use corrosion reconstruction synthesis techniques to guide the preparation of efficient and stable electrocatalysts. Herein, the most recent developments in electrocatalyst corrosion chemistry are outlined, including corrosion mechanisms, mitigation strategies, and corrosion syntheses/reconstructions based on typical materials and important electrocatalytic reactions. Finally, potential opportunities and challenges are also proposed to foresee the possible development in this field. It is believed that this contribution will raise more awareness regarding nanomaterial corrosion chemistry in energy technologies and beyond.

Biological Matrix Supply Chain Shortages: More Matrices Are Now Rare-the Case for Surrogate Matrices.

The COVID-19 pandemic has strained the biological matrix supply chain. An upsurge in demand driven by numerous COVID-19 therapeutic and vaccine development programs to combat the pandemic, along with logistical challenges sourcing and transporting matrix, has led to increased lead times for multiple matrices. Biological matrix shortages can potentially cause significant delays in drug development programs across the pharmaceutical and biotechnology industry. Given the current circumstances, discussion is warranted around what will likely be increased use of surrogate matrices in support of pharmacokinetic (PK), immunogenicity, and biomarker assays for regulatory filings. Regulatory authorities permit the use of surrogate matrix in bioanalytical methods in instances where matrix is rare or difficult to obtain, as long as the surrogate is appropriately selected and scientifically justified. Herein, the scientific justification and possible regulatory implications of employing surrogate matrix in PK, immunogenicity, and biomarker assays are discussed. In addition, the unique challenges that cell and gene therapy (C>) and other innovative therapeutic modalities place on matrix supply chains are outlined. Matrix suppliers and contract research organizations (CROs) are actively implementing mitigation strategies to alleviate the current strain on the matrix supply chain and better prepare the industry for any future unexpected strains. To maintain ethical standards, these mitigation strategies include projecting matrix needs with suppliers at least 6 months in advance and writing or updating study protocols to allow for additional matrix draws from study subjects and/or re-purposing of subject matrix from one drug development program to another.

Perovskite Solar Cells Employing a PbSO4(PbO)4 Quantum Dot-Doped Spiro-OMeTAD Hole Transport Layer with an Efficiency over 22.

2,2',7,7'-Tetrakis(N,N-di-p-methoxyphenyl-amine)-9,9'-spirobifluorene (spiro-OMeTAD), the most widely used hole transport material in high-efficiency perovskite solar cells (PSCs), still has serious defects, such as moisture absorption and poor long-term conductivity, which seriously restrict further improvement of the power conversion efficiency (PCE) and stability of the cell. Herein, to overcome these problems, inorganic salt PbSO4(PbO)4 quantum dots (QDs) are incorporated into spiro-OMeTAD as the hole transport layer (HTL) for the first time. The incorporated PbSO4(PbO)4 QDs significantly hinder the agglomeration of lithium bis(trifluoromethanesulfonyl)-imide and improve the long-term conductivity through the oxidative interaction between PbSO4(PbO)4 QDs and spiro-OMeTAD and hydrophobicity of the HTL. Furthermore, the spiro-OMeTAD:PbSO4(PbO)4 composite film can effectively passivate perovskite defects at the perovskite/HTL interface, resulting in suppressed interfacial recombination. As a result, the PSC based on the spiro-OMeTAD:PbSO4(PbO)4 HTL shows an improved PCE of 22.66%, which is much higher than that (18.89%) of the control device. PbSO4(PbO)4 also significantly improves the moisture stability for 50 days at room temperature (at RH ∼ 40-50%) without encapsulation. This work indicates that inorganic PbSO4(PbO)4 QDs are crucial materials that can be employed as an additive in spiro-OMeTAD to enhance the efficiency and stability of PSCs.