From the perspective of sustainable energy and green hydrogen, the critical challenge in seawater electrolysis lies in suppressing competitive chloride oxidation and corrosion at the anode. Despite the proposed protection mechanism based on surface reconstruction-derived anion repellence, a fundamental question of selectivity remains: why does the protective layer exclude Cl- but not the formally equivalent OH-? We now redefine the connection between reconstruction and interfacial protection in NiFeS anodes to elucidate the origin of underlying selectivity. In-situ Raman, in-situ X-ray absorption spectroscopy, and molecular dynamic calculations further confirm that the reconstructed SO42- establishes an enhanced hydrogen-bond network. This network significantly weakens the hydrogen-bonding strength of Cl- relative to H2O, thereby enhancing the discrimination between OH- and Cl-. In practical application, NiFeS demonstrates energy-saving seawater splitting performance (261.8 mV @ 100 mA·cm-2), long-term durability (2000 h @ 1.0 A·cm-2), and enables stable intermittent electrolysis (1500 start-stop cycles @500 mA·cm-2). When integrated into an anion exchange membrane cell, it shows promising electrolysis performance for industrial applications (1.970 V @ 1.0 A·cm-2).

Volatile organic compounds (VOCs) from industrial sources exhibit complex compositional diversity, encompassing various components such as aromatic hydrocarbons and halogenated hydrocarbons; therefore, high-performance adsorbent materials must possess co-adsorption capability for different VOCs. Carbon-based adsorbent owns potential for simultaneously removal of diverse pollutants due to their tunable multiscale structures, which requires constructing hierarchical functional zones to improve co-adsorption thermodynamics and kinetics of different VOCs molecules. Compared to widely-focused equilibrium adsorption capability, co-adsorption kinetics carbon adsorbents before breakthrough stage (C/C-0 < 0.1) which is a critical indicator for practical adsorption craft, have received little attention. Herein, we find that integrating metal sites with hierarchical pore of activated carbon can simultaneously improve equilibrium and breakthrough adsorption capacities of activated carbon adsorbent. Compared to microporous activated carbon, hierarchical porous carbon with metal site decoration demonstrates a 324 mgg(-1) increase in equilibrium co-adsorption capacity for toluene and dichloromethane. Particularly, breakthrough time of weakly adsorbed dichloromethane can be extended by 138 %, leading to a 132 mgg(-1) enhancement in co-adsorption capacity before breakthrough stage. Simulation results indicate that improved co-adsorption kinetics are primarily attributed to enhanced electrostatic interactions with dichloromethane. This study provides a new strategy for improving co-adsorption of multiple pollutants in practical adsorption craft.

Pyrolysis is an essential process for coal conversion to carbon-based materials, the regulation of which is limited by the rigid skeleton and low active components in coal. Co-pyrolysis of plastic and coal have been validated to be an efficient strategy to adjust coal thermochemical conversion behavior, however, specific regulatory effects on physicochemical properties of solid pyrolytic carbon remain to be revealed. Herein, the role of typical plastic component PET addition in coal pyrolysis was systematically explored. Thermogravimetric analysis under N2 and O2 atmospheres showed that the addition of 20 wt% PET not only increased the relative carbon yield, but also exhibited the lowest apparent activation energy of 103.31 kJ mol-1. XRD and Raman characterization revealed that the addition of PET increased the formation of pseudo graphite phases with a loose graphite like microcrystalline structure by 10.58 %. FTIR and EPR characterization further revealed that the synergistic enhancement of aromatization process and defect density originated from polar free radicals derived from PET. These radicals promoted the cleavage of weak bonds in coal, generating active sites for aromatic layer growth, and simultaneously depleted [H] in the system, inhibiting the cracking of aromatic structures and the healing of defects.

Efficient mass transfer of reactant or product is an essential process for heterogeneous catalysis cycle in porous catalyst, which ensures timely recovery of reaction vessel and long-term stability. Taking SO2 catalytic removal by porous carbon as an example, the removal efficiency and capacity is limited by the mass transfer behavior of product H2SO4 in nanometer-sized porous channel. Herein, based on multi-scale modelling combining density functional theory (DFT), grand canonical Monte Carlo (GCMC) and molecular dynamic (MD) simulation, we found that coupling of surface hydrophilic oxygen group with hierarchical pore can efficiently enhance the mass transfer behavior of product H2SO4, thereby improving overall catalytic process. For the hierarchical pore configuration with 0.7 nm confined space matched to nanometer-sized slit pore, the hydrophilic oxygen group in 0.7 nm reaction vessel is essential for H2O local enrichment to induce H2SO4 mass transfer from surface active site to confined space; the coupling between hydrophilic oxygen group and slit pores with sizes in 1.0-1.5 nm range can provide mobile H2O to further carry out product H2SO4 away from 0.7 nm reaction vessel, increasing H2SO4 self-diffusion coefficient by nearly one order of magnitude compared to that in sub-nanometer confined space. By comparing H2SO4 mass transfer in different types of hierarchical pore, hierarchical structure with 0.7 nm reaction vessel matched to 1.0 nm-sized slit pore that contains 3.9 at% hydrophilic oxygen group is found to own the strongest mass transfer ability for H2SO4, and the calculated H2SO4 self-diffusion coefficient is as high as 3.9 x 10-6 cm2 s- 1 . Above observed the enhancement of H2SO4 mass transfer was further validated by desulfurization experiment using model porous carbon. This work for the first time reveals coupling effects of surface oxygen group and pore configuration on product mass transfer during SO2 catalytic removal by porous carbon, and obtained conclusions about confined mass transfer can also provide guidelines for heterogeneous catalysis in other porous catalysts.

Volatile organic compounds (VOCs) are important sources of air pollution complex in China and exist as mixtures of different-sized components in industrial exhaust gases. Activated carbon is a type of widely-used adsorbent for VOCs removal, but faced with poor VOCs co-adsorption performance due to competitive adsorption. Herein, an efficient strategy of constructing hierarchical pore configuration was proposed to alleviate competitive adsorption of VOCs with different kinetic diameters and further enhance co-adsorption capacity. The role of hierarchical pore configuration in co-adsorption of typical VOCs toluene and dichloromethane was revealed based on coal-based porous carbon with tunable pore hierarchy. Dynamic adsorption experiments show that micropore-dominant carbon, adsorption capacities of toluene and dichloromethane under co-adsorption dramatically decreased by 14% and 42% respectively compared to single component adsorption. However, the loss of adsorption capacity within the hierarchical porous carbon was only 9% and 14% under the same conditions. Correlation analyses and molecular dynamics simulations showed that hierarchical porous carbon could induce unique adsorption behavior in which toluene tends to be stored in mesopore and dichloromethane is mainly distributed in micropore, thus effectively reducing the competitive adsorption. Guided by the found mechanism, we further prepared hierarchical porous carbon with high specific surface area and pore volume, based on which adsorption capacity of toluene and dichloromethane under co-adsorption condition was enhanced by more than 50% compared to micropore-dominant carbon. The relevant mechanism provides a theoretical basis for advancing the optimization of co-adsorption process of mixed VOCs.

In the thermochemical sulfur–iodine water splitting cycle for hydrogen production, the hydrogen iodide (HI) decomposition reaction serves as the rate-determining step, and its high efficiency relies on the precise design of active sites on the catalyst. This paper combines experimental characterization with density functional theory (DFT) calculations, focusing on activated carbon catalysts. By regulating the types and contents of oxygen-containing functional groups through H2 reduction treatment at different temperatures, the influence of oxygen-containing functional groups on HI decomposition was investigated. The results show that H2 reduction treatment can gradually remove oxygen-containing functional groups such as carboxyl, hydroxyl, and carbonyl groups on the surface of activated carbon without significantly affecting the pore structure. Catalytic activity tests conducted under the typical reaction temperature of 500 °C confirmed that as the content of oxygen-containing functional groups decreases, the HI decomposition efficiency increases. DFT calculations further revealed the role of oxygen-containing functional groups: they inhibit the chemisorption of reactant HI on unsaturated carbon atoms and alter the desorption activation energy of product H2, thereby affecting the overall reaction process. This study provides important theoretical guidance and experimental basis for designing efficient HI decomposition catalysts.

Direct seawater electrolysis offers a sustainable route to producing green hydrogen, but it suffers from severe chloride corrosion at conventional anodes. Challenging the long-standing electrostatic repulsion model for chloride suppression, we reveal that interfacial hydrogen-bond networks govern selective OH- transport while excluding Cl-. Through integrated ab initio molecular dynamics and in situ Raman spectroscopy, we demonstrate that structured water layers near the anode form a dynamic H-bond sieve: OH- undergoes barrier-free transfer by reconfiguring the H-bond network, while Cl- faces high rejection due to its inability to reorganize interfacial water. Leveraging this mechanism, we engineer an interfacial H-bond buffer using SO42- and CO32- anions. SO42- reinforces the H-bond network to block Cl-, while CO32- acts as an OH- pump to mitigate depletion at high current densities. The optimized buffer enables a CoFe LDH anode to achieve exceptional activity (overpotential of 291.4 mV at 300 mA cm-2) and stability (550 h at 2.0 A cm-2). When integrated into an anion-exchange membrane electrolyzer, the system delivers industrially relevant performance (2.51 V at 1.0 A cm-2, 4.85 kWh Nm-3 H2) with 1000 h stability. This work establishes a transformative H-bond-mediated ion-sieving paradigm for corrosion-resistant seawater electrochemistry.

Nanoscale pores and heteroatom dopants in metal-free carbon catalysts are essential functional units serving as mass transport channels and catalytic sites of reactants, respectively, for achieving NOr selective catalytic reduction with NH3 (NH3-SCR). Existing studies have confirmed the positive impact of nitrogen dopants on enhancing catalytic activity, but the changes in pore topology (micropores or hierarchical pores) and their coupling effect with doping sites are still unclear. Here, we for the first time unveil the coupling interaction between nitrogen dopants and pore topology using model carbon catalysts with adjustable pore configurations and doping environment. Dynamic experiments indicate that for the undoped carbon, the hierarchical porous carbon delivers higher NOr conversion relative to the single microporous carbon, which is attributed to the rapid mass transfer of meso-/macropores, as confirmed by numerical simulations. However, for the nitrogen-doped carbon, the nitrogen-rich microporous carbon (NMAC-MW) demonstrates the highest NOr conversion (90 % at 160 degrees C with the weight hourly space velocity of 4000 mL g-1 h-1). Density functional theory calculations and in-situ characterizations reveal that nitrogen species switch reaction pathways from the standard NH3-SCR to the fast NH3-SCR and then couple the confinement effect of micropores to boost O2 activation, ultimately promoting the NH3-SCR. This work offers insights into the multi-scale engineering of effective carbon catalysts for NOr removal.

Carbon-based catalysts offer a cost-effective solution for VOC catalytic removal, featuring abundant porosity that enables the dispersion of metal active sites. This study presents a facile synthesis protocol for activated carbon (AC) supported Mn/Ce oxide catalysts, revealing the significant role of N-doping in enhancing toluene catalytic oxidation. During the activation process, the incorporation of Mn/Ce salts into carbon precursor (coal) promoted the formation of micropore and graphitic structure in resultant ACs, whilst Mn/Ce salts were converted to oxide nanoparticles uniformly distributed on the carbon surface. Additionally, the introduction of a nitrogen source (EDTA) resulted in 4.0 at.% N doping within the carbon matrix, including 1.44 at.% pyridinic-N. At 250 degrees C and 300 degrees C, the N-doped AC exhibited toluene removal efficiencies of 90.1 % and 95.4 %, respectively, with decent thermal stability and resistance to irreversible sulfur (SO2) poisoning. In-situ DRIFTS, O2-TPD, and XPS analysis confirmed that N-doping boosted O2 activation on the carbon surface, facilitating toluene oxidation via the L-H (Langmuir-Hinshelwood mechanism), and promoting the restoration of oxygen vacancy in Mn/Ce oxides through the MvK (Mars-van Krevelen) mechanism. These findings provide new insights into the synergistic interactions between N-doping sites on carbon supports and metal active sites, highlighting their combined role in the catalytic oxidation of toluene.

Low-temperature selective catalytic reduction of NOr using NH3 (NH3-SCR) over metal-free carbon catalysts significantly relies on the precise engineering of active sites. Although heteroatom dopants have been proven to be active sites, the effects of intrinsic defects in carbon catalysts and their coupling with heteroatoms on the NH3-SCR pathway are still unclear. Here, we demonstrate a novel approach to boosting NH3-SCR through the synergy between nitrogen dopants and vacancies, achieved by preparing carbon catalysts with controllable nitrogen-doping and vacancy sites. The introduction of enriched vacancies and nitrogen dopants by a microwave-induced co-activation method provides a superior NOr conversion (100 % at 180 degrees C) and good sulfur resistance. Density functional theory (DFT) calculations further unlock the coupling effects of nitrogen dopants and vacancies, that vacancies can not only distort the carbon basal plane and redistribute charges, thereby enhancing O2 activation, but also activate the originally inert pyridine nitrogen and synergistically enhance O2 activation. In this way, NO oxidation to NO2 can be promoted, further enabling the occurrence of the fast NH3-SCR pathways (NO + NO2 + 2NH3 -> 2N2 + 3H2O), which is crucial for improving the efficiency of NOr removal. This work provides new perspectives on the role of vacancies in carbon-catalyzed reactions, guiding the design of highperformance carbon catalysts for cost-effective NOr removal.

Carbon material is a type of promising adsorbent for flue gas CO2 capture, where micropore and dopants are key functional units and intertwined with each other. Due to the difficulty in detaching micropore and functional sites, their effects on CO2 adsorption are still in debate. Herein, we unravel coupling effects of micropore confinement and functional sites combining machine learning (ML) and multi-scale simulations. High-throughput Grand Canonical Monte Carlo (GCMC) simulations in combination with density functional theory (DFT) calculations clarify that CO2 adsorption mechanism under pore-dopant coupling is dependant on both micropore confinement environment and interaction type of CO2 with functional sites. For basic dopants owning chemical interactions with CO2, adsorption potential driven by Lewis acid-base interactions dominate CO2 adsorption behavior and the optimal pore size is distributed at 7 Å. For dopants that predominantly adsorb CO2 by physisorption interaction, steric effect becomes a key factor influencing CO2 adsorption behavior, which will result in a shift in optimal pore size for CO2 adsorption from 7 to 8-10 Å and alter adsorption selectivity. In this case, new descriptor free volume (Vf) was identified to describe coupling effects of micropore and functional sites. Guided by theoretical findings, we prepare carbon adsorbent with both heteroatom dopants and enlarged pore size, which exhibits leading-level CO2 adsorption capacity of 4 mmol g−1 at ambient condition, 130% higher than that without pore size optimization. This work demonstrates crucial role of micropore-dopant coupling mode on CO2 adsorption, and provides new direction of developing high-performance carbon adsorbent beyond traditional standalone pore or doping engineering.

BackgroundThe current investigation examines the association between artificial sweetener (AS) consumption and the likelihood of developing chronic kidney disease (CKD), along with its impact on kidney function.MethodsWe utilized data from the National Health and Nutrition Examination Survey from 2003–2006 to conduct covariance analysis and weighted adjusted logistic regression, aiming to assess the association between artificial sweetener intake and CKD risk, as well as kidney function indicators. Subsequently, we employed Mendelian randomization methods to validate the causal relationship between the intake of artificial sweeteners, CKD risk, and kidney function indicators. Instrumental variable analysis using inverse-variance weighting and Robust adjusted profile score were the primary analytical methods employed.ResultsA total of 20,470 participants were included in the study, with 1,257 participants ultimately included in the analysis. In all adjusted logistic regression models, no significant association was found between the intake of artificial sweeteners and CKD risk. Similarly, the summary odds ratios (OR) for each unit change in genetically predicted CKD risk were 2.14 (95% CI: 0.83, 5.21, p = 0.092), 1.41 (95% CI: 0.54, 3.63, p = 0.482), and 1.50 (95% CI: 0.50, 4.52, p = 0.468) for the impact of artificial sweeteners added to cereals, tea, and coffee, respectively. It was only observed that adding artificial sweeteners to coffee was associated with a modest reduction in urinary albumin-to-creatinine ratio (OR = 0.94, 95% CI: −0.108, −0.022, p = 0.003), the effect appeared to be relatively small and may not directly impact the individual level.ConclusionOur study does not support a causal relationship between artificial sweetener intake and the risk of CKD. However, due to the limitations and potential confounding factors, these findings need to be further validated through larger sample sizes in observational studies and Mendelian randomization analyses.

Rising the activity of activated carbons by surface modification has attracted considerable research attention in the fields of gas adsorption and energy storage. However, conventional functionalization of activated carbons typically requires high cost and long-term heating process. In this work, we report a simple and feasible strategy to prepare N-rich activated carbons with well-developed porosities through microwave heating. Through microwave heating, N-rich (up to 9.35 at.%) activated carbons with high porosities can be prepared within 20 min, reducing preparation time and energy consumption by 77.0% and 99.4%. Under microwave irradiation, the interaction between melamine and carbon precursors is promoted to generate an amount of defects, resulting in the introduction of N species and reducing the consumption of nitrogenous reagents (50%). Moreover, due to the enhanced van der Waals interactions between the nitrogenous carbon surface and molecules, the prepared N-rich activated carbons present excellent increase in breakthrough adsorption capacity of toluene (up to 26.0 %) and CO2 uptake (9.8 %) with similar pore structure. In summary, this study provides a facile, efficient, and universal strategy for surface modification of activated carbons toward a range of applications.

The increasingly stringent exhaust emission standards of stationary and mobile sources have sparked significant interest in developing catalysts for NOx selective catalytic reduction with NH3 (NH3-SCR) at low temperatures (<300 °C). Therein, the porous catalyst with a unique ability in reactant adsorption and enrichment is an elegant solution for low-temperature NH3-SCR. Due to the cross-scale reaction pathway involving both nanopore and active sites in porous catalysts, mass transfer acts as a prerequisite process and plays a pivotal role in low-temperature activity. However, a systematic understanding of mass transfer behavior in low-temperature NH3-SCR remains to be established. Here, we review porous low-temperature catalysts from a new perspective that highlights the role of mass transfer. This review starts with an introduction to the basic characteristics of porous catalysts and the heterogeneous catalysis process in porous catalysts to emphasize the importance of mass transfer behaviors. Afterward, various effects of mass transfer including the active site accessibility, the reaction micro-environment, and the working life on the overall reaction, as well as corresponding strengthening methods are reviewed. Finally, issues and perspectives on the future development direction of porous catalysts for NH3-SCR are proposed. We hope that this review can provide helpful guidance for designing high-performance porous catalysts for low-temperature NH3-SCR.

Microwave heating for the production of activated carbons has garnered significant research interest in the realms of gas adsorption. Nonetheless, the effect of tunable-energy-density microwave irradiation on the production of activated carbons is unclear. Herein, we report a tunable-energy-density microwave heating strategy to rapidly prepare highly microporous activated carbons. With the raising microwave energy density, the pore volume increases from 0.68 cm3·g−1 to 0.89 cm3·g−1, with a 70% decrease in the preparation time. Moreover, due to the high ratio of micropore (84.4%–86.6%) and great hydrophobicity, the optimal toluene adsorption capacity reaches 0.56 g·g−1 and 0.47 g·g−1 in the dry and wet (97% RH) environment, respectively. Due to the high ratio of ultramicropore (62.6%–69.0%), at 1 bar, the optimal CO2 uptake for 25 °C and 0 °C reaches 4.27 mmol·g−1 and 6.41 mmol·g−1, respectively. This study introduces a straightforward and effective method for the swift production of activated carbons, applicable across a spectrum of uses.

Activated carbon is an important adsorbent for the adsorption removal of water or gas pollutants due to its low cost, high efficiency, and large-scale production potential; however, currently commercial activated carbon prepared through physical or chemical activation commonly shows a single microporous characteristic, making it difficult to match different kinds of pollutants. Here, we propose a convenient and cost-effective pore regulation strategy by introducing a trace carbonate catalysis process into the activation reaction, in which we find that the types of cations (Na, K, Ca) in carbonate have a significant impact on the pore topology of coal-based activated carbon, further revealing the role of cation induced catalytic gasification in pore regulation. Therein, K and Ca enhance the formation of micropores and meso-/macropores respectively, while Na promotes the pore development across the entire size range resulting in a hierarchically porous structure with high specific surface area. Kinetic analysis, density functional theory calculations, and three-dimensional pore fractal network characterization reveal that the pore development is collectively determined by the gasification reaction rate and depth. Evaluated as adsorbents, the obtained NaAC sample by Na catalysis demonstrates excellent adsorption capacities for both small-molecule toluene (467 mg g-1) and large-molecule tetracycline (374 mg g-1). This work for the first time elucidates the cation-induced gasification effect and provides a simple and cost-effective method for regulating the pore topology of activated carbon with only trace catalyst dosage.

Heteroatom doping is essential for enhancing the performance of activated carbons (ACs) in various environmental-related applications. Herein, a scalable confined-space microwave heating (CSMH) strategy is proposed and demonstrated to achieve minute-level fast preparation of N/O co-doping ACs with well-developed porosity. The introduction of confined space prevents the escape of nitrogenous and oxygenous volatiles, enabling the sufficient reaction for heteroatom doping. Therefore, the nitrogen content of MWC-0.5 (6.0 at.%) is higher than that of MW-0.5 (3.5 at.%) and CH-0.5 (4.3 at.%). This causes a nearly 50% reduction in the consumption of nitrogenous reagents. Moreover, through CSMH strategy, N/O co-doped ACs (6.0 at% and 8.1 at% for N and O, respectively) with high pore volume (0.53 cm3·g-1) can be acquired to achieve an excellent adsorption performance for toluene (0.31 g·g-1) and CO2 (3.97 mmol·g-1 at 25 °C and 1 bar) and outstanding CO2/N2 selectivity (189 at 0.02 bar). This work for the first time develops a scalable confined-space N/O co-doped strategy for enhancing the chemical activity of ACs with low-spend nitrogenous reagents.

Activated coke is a type of commonly used adsorbent for benzene series VOCs such as toluene, but traditional microporous activated coke usually faces the challenge of poor regeneration performance. Herein, based on self-made activated cokes with typical pore configuration, we found that adsorption and regeneration of toluene can be simultaneously enhanced by constructing hierarchical pore in activated coke. Correlations of pore configuration with toluene adsorption capacity and regeneration efficiency reveal that micropore contributes for strong toluene adsorption; meso-macropore provides mass transfer channel for toluene desorption and regeneration process. Hierarchical porous activated coke prepared from Zhundong subbituminous coal not only achieves the highest toluene adsorption capacity of 340.92 mg·g−1, but also can retain more than 90

目的 系统评价雷公藤多苷联合血管紧张素转换酶抑制剂或血管紧张素Ⅱ受体阻滞剂治疗糖尿病肾病的有效性和安全性.方法 检索相关随机对照试验,根据纳入排除标准进行文献筛选,并对其进行方法学质量评价及荟萃分析.结果 共纳入 24 篇文献,2171 例糖尿病肾病患者.与对照组相比,试验组可明显提高临床疗效[OR=3.13,95%CI(2.26,4.33),P<0.00001],降低 24 h尿蛋白[MD=-0.69,95%CI(-0.83,-0.56),P<0.00001]、血肌酐[MD=-7.90,95%CI(-15.34,-0.45),P=0.04]、血尿素氮[MD=-0.34,95%CI(-0.65,-0.04),P=0.03],升高血清白蛋白[MD=3.44,95%CI(2.29,4.59),P<0.00001],改善患者空腹血糖[MD=-0.19,95%CI(-0.29,-0.08),P=0.0008],但糖化血红蛋白两组间无统计学差异(P=0.05).不良反应发生率方面,试验组高于对照组[RD=0.03,95%CI(0.00,0.06),P=0.04].结论 雷公藤多苷联合血管紧张素转换酶抑制剂/血管紧张素Ⅱ受体阻滞剂治疗糖尿病肾病,在临床疗效、肾功能及空腹血糖方面优于单独应用血管紧张素转换酶抑制剂/血管紧张素Ⅱ受体阻滞剂.