Direct air capture (DAC) of CO2 is pivotal for mitigating climate change, with moisture-swing adsorbents emerging as an energy-efficient approach to this end. Herein, we report ultra-high capacity quaternized polyethylene terephthalate (QPET) adsorbents fabricated via ultraviolet-induced grafting of quaternary ammonium groups onto PET substrates. The resulting QPET fabric exhibits a remarkably high adsorption capacity of 6.08 mmol/g under ambient conditions, which is 1.64 times that the prior record (3.71 mmol/g) for moisture-swing adsorbents, and is over 6 times that of the most-studied resin-based adsorbents. This exceptional performance is attributed to the high density of grafted quaternary ammonium groups and the intrinsic three-dimensional fibrous network of the PET fabric substrate, which provide abundant CO2 adsorption sites and gas diffusion channels. The adsorbent demonstrates excellent cyclic stability, retaining consistent adsorption/desorption capacities across three full cycles and ten short-term cycles. Furthermore, its moisture-driven regeneration mechanism obviates the need for thermal or pressure inputs, while the utilization of low-cost PET substrates enhances scalability. This work provides a promising strategy for developing high-performance, cost-effective adsorbents tailored for large-scale CO2 capture from ambient air.

Rational design of high-entropy intermetallic compounds (HEICs) remains challenging due to complex structure-property relationships and the lack of predictive tools. Here, a data-driven framework is presented to evaluate the hydrogen evolution reaction (HER) activity of L1 2 -type quinary Pt 3 M(4) HEICs, where M comprises any four elements from six 3 d transition metals (Cr, Mn, Fe, Co, Ni, Zn). Guided by the Pm-3m space group, 15 distinct compositions with numerous microstates are designed. A deep neural network, trained on 453 computed datasets, predicts hydrogen adsorption energy (∆ E H* ) across 20 000 microstructures per composition, enabling statistical mapping of site-specific performance. To capture the effect of local atomic environments, a novel statistical evaluation approach is introduced that quantifies the number of microstates falling within the optimal ∆ E H* range, advancing beyond conventional mean-based evaluations. Among all candidates, Pt 3 (CrMnFeCo) emerges as the most promising HER catalyst, validated experimentally over a wide pH range. Further in-depth data mining reveals that surface Co, Cr, and Fe optimize Pt-Pt-M sites, while subsurface Ni and Co modulate Pt-Pt-Pt interactions. This study establishes a new paradigm for HEIC catalyst design and deepens the mechanistic understanding of activity origin in complex multimetal systems.

Inverse design of solid-state materials with desired properties remains a central challenge in materials science, requiring exploration of vast chemical spaces containing potentially 10100 possible structures. Current generative approaches face limitations in computational efficiency, multi-property targeting precision and mechanistic interpretability. Here, we introduce MatterGPT, an autoregressive Transformer-decoder architecture that leverages SLICES (Simplified Line-Input Crystal-Encoding System) representation to generate novel crystals through conditional next-token prediction. Trained on 306,533 crystal structures, MatterGPT achieves > 99% structural validity, > 99% structural uniqueness and > 50% novelty rates while targeting both specific lattice-insensitive and lattice-sensitive properties. Critically, MatterGPT enables direct multi-property generation without post-generation filtering. Interpretability analysis reveals clear property-guided generation mechanisms and systematic chemical space exploration. The comprehensive open-source release, including MatterGPT Hub integration platform, establishes sequence-based autoregressive generation as a computationally efficient and interpretable paradigm for inverse crystal design, accelerating materials discovery across energy storage, electronics, and functional applications.

Geckos in nature can shed their tails via autotomy to distract predators and escape, while soft robotics, despite its flexibility, lacks detachable and reconfigurable components. This work introduces a surface buckling enabled soft clutch that achieves bidirectional (normal and tangential) engagement through geometric interlocking of pre-programmed inverted trapezoidal waveforms on stretchable substrates. The clutch design leverages compressive stress-driven buckling of thin films to create reversible morphological transitions. Experimental results demonstrate that the soft clutch achieves stable tensile and shear strengths. Reduced angle between the film legs and the substrate and increased film thickness improve mechanical performance of the soft clutch. Theoretical models incorporating film buckling and geometric constraints accurately predict tensile and detachment strengths. A bio-inspired gecko robot with a clutch-connected detachable tail validated the clutch's utility: under simulated predation, pneumatic actuation enabled tail autotomy, ensuring escape of the body part.

Traditional petrochemical-derived plastics are challenging to recycle and degrade, and the existing (re)process methods are organic solvent-based and/or energy-intensive, resulting in significant environmental contamination and greenhouse gas emissions. This study presents a sustainable bioplastic material characterized by multi-closed-loop recyclability and water (re)processability. The bioplastics are derived from abundant polysaccharide sources of dextran, alginic acid, carboxymethyl cellulose, and DNA of plant and living organism waste. The process involves chemical oxidation of polysaccharides to produce aldehyde-functionalized derivatives, which subsequently form reversible imine covalent bonds with amine groups in DNA. This reaction yields water-processable polysaccharide/DNA crosslinked hydrogels, serving as raw materials for producing sustainable bioplastics. The bioplastic products exhibit (bio)degradability and recyclability, enabling aqueous recovery of the hydrogel constituents through plastic hydrolysis and the natural biodegradability of DNA and polysaccharides. These products demonstrate excellent resistance to organic solvents, self-healing, scalability, and effective processing down to nanometer scales, underscoring their potential for broad and versatile applications. The work provides potential pathways for advancing sustainable and environmentally friendly bioplastic materials.

The size effects were experimentally investigated and the underlying mechanism was analyzed. The results reveal that, as the specimen size increases, the interconnectivity of macropores slightly decreases. This in turn constrains the diffusion of CO2 and moisture in the specimens, resulting in an increase in the discrepancy between the internal and external carbonation degrees. An increase in cement paste thickness simultaneously decreases the quantity, average size, and interconnectivity of macropores, lowering the diffusion efficacy of CO2 and moisture and exacerbating the overall heterogeneity in carbonation. Moreover, the gradual blockage of macropores leads to the emergence of localized ‘occluded zones’ with much lower carbonation degree. The reduction in aggregate size significantly alters the average diameter and connectivity of macropores. leading to notable change to overall non-uniformity. This study provides insight into improving the CO2 curing effect of pervious concrete products and developing uniform curing methods.

Direct air capture (DAC) of CO2 is an important technology to mitigate mobile carbon emissions, reduce atmospheric CO2 concentration, and cope with climate change. Moisture-swing adsorption is regarded as one of the most promising technologies in DAC due to its low energy consumption and ease of operation. In this work, a cheap and easily available moisture-swing adsorbent of potassium carbonate loaded on porous supports (i.e., activated carbon, magnesium oxide, and zeolite) was prepared for CO2 capture from ambient air. The composite adsorbent of potassium carbonate on activated carbon showed the best performance with a DAC capacity of 0.562 mmol/g at 25 degrees C and 5% relative humidity. The effects of temperature, relative humidity, and CO2 concentration on the adsorption performance were investigated systematically, as well as the cyclic DAC performance. In 50 adsorption-desorption cycles, the adsorption capacity of the composite adsorbent decreased by similar to 40% due to potassium carbonate leaching loss during water evaporation but can be fully recovered simply by re-impregnating with potassium carbonate again.

Direct air capture (DAC) of CO2 is emerging as an important technology to mitigate the environmental challenges posed by excessive carbon emissions. The development of reliable and affordable adsorbents has long been a topic of great interest in the DAC field. In this work, through a quaternization process, inexpensive and readily available plant-based biochars including walnut shell, cornstalk, rice husk, and long-stalked lentil shell were prepared as moisture-swing adsorbents to capture CO2 from ambient air. Among these biochar adsorbents, the most effective one was found to be the quaternized long-stalked lentil shell, whose CO2 adsorption capacity reached 0.88 mmol/g at 25 degrees C and 50% relative humidity, which is around five times that of previously reported biochar moisture-swing adsorbents (including bamboo cellulose and chitosan aerogel). Interestingly, different from the anion-exchange resin (the most studied moisture-swing adsorbent) whose adsorption capacity decreases progressively with increasing ambient humidity and the optimal adsorption requires a relative humidity below 5%, the adsorbents developed here obtained optimal adsorption performance at 50% relative humidity (at room temperature). This result greatly expands the suitable deployment area of moisture-swing DAC since the relative humidity of most land areas on earth is in the range of 40-80%.

Poor O2 tolerance and high reaction temperature of the conventional oxygen carriers challenge the direct utilization of impure CO2 via chemical looping. Here, Pt-Ni bimetallic Ce-based oxygen carriers with excellent O2 tolerance are developed for highly efficient reduction of O2-containing CO2 at low temperatures. At a temperature as low as 700 °C, high CO2 conversion (≈92%) is obtained over 0.1 wt% Pt-0.1wt% Ni/CeO2 oxygen carrier in the CO2 feed gas with 16.7% O2 impurities. These results benefit from that Pt-Ni bimetal plays a crucial role in improving CH4 partial oxidation and accelerating the breaking of the C═O bond to alleviate the competitive oxidation of O2 impurities. Ni compensates for the reduction of low-temperature redox activity caused by the decrease of Pt content. Moreover, Pt-Ni/CeO2 oxygen carriers exhibit excellent structural and performance stability during redox cycles. This work presents a feasible strategy for the direct utilization of impure CO2 at low temperatures and realizing a carbon-neutral cycle.

Mechanically activated nanolithia can be fully decomposed during the first charge half-cycle and offers a high prelithiation capacity up to 1200 mA h g −1 at 4.3 V ( vs. Li + /Li) upper cutoff voltage.

Metal phthalocyanines molecular catalysts exhibit the unique ability of CO2 electrochemical reduction reaction (CO2ERR) thanks to their well-defined macrocycle structure. In this work, we introduced different substituting functional groups at the phthalocyanine ring of cobalt phthalocyanine to study the relationship of molecular structure optimization and CO2ERR activity. An optimal nitro-substituted cobalt phthalocyanine catalyst can mediate CO2 to CO in a H-cell with maximum selectivity of similar to 94% together with a current density of 12.6 mA cm(-2) at -0.877 V vs. RHE. The insights of this work on designing and optimizing of the molecular catalysts contribute to lower energy as well as cost-effective CO2ERR.

Noble-metal-free semiconductor composites are very valuable for efficient water splitting driven by visible light. In this paper, CdS@Ni2P was successfully prepared by a simple hydrothermal method followed by in situ photodeposition. The results showed that the best photocatalytic hydrogen production rate of the composite is 287 mu mol h(-1), which is about 98.3 times that of pure CdS. The high activity of the material may be attributed to the intimate interface between the Ni2P cocatalyst and CdS nanorods for accelerating the separation and transport of photoelectrons. Further UV and PL tests found that Ni2P significantly extends the lifetime of photogenerated charge carriers and reduces charge recombination rates, resulting in improved photocatalytic H-2 production performance. The potential mechanism of photocatalytic enhancement of CdS@Ni2P composite samples was proposed based on the experimental results and DFT calculation, which could lead to a neoteric approach for the efficient preparation of other photocatalytic materials.

With the mission of negative emission, moisture swing sorbents are developing fast in recent years, thanks to their low energy consumption and simple operating system. The sorbent was proposed to capture CO2 directly from ambient air, while its low energy-cost nature underpins carbon capture from a variety of other gas streams with larger CO2 concentrations. The present study exploits the moisture swing process for capturing industrial process CO2, and the CO2 removal from natural gas is used for demonstration. Compared to capturing CO2 from the air, the adsorption capacity is promoted significantly as the CO2 concentration in the gas mixture is much higher (1-20%). A stable cyclic capacity with -1.0 mmol/g is obtained, which is comparable to that of aqueous/solid amine sorbents. Moreover, a moisture swing process flow is developed for CO2 removal from natural gas, and an energy consumption analysis of the moisture swing process is conducted with comparison to the traditional amine scrubbing technique. We find that the energy consumption of the moisture swing decarbonization process (-187.38 kJ/Sm3) is less than half that of the methyl diethanolamine solution method (954-1304 kJ/Sm3), which strongly supports the moisture swing process as a promising method for capturing industrial process CO2. (c) 2021 Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

International Center for Applied Mechanics, State Key Laboratory for Strength and Vibration of Mechanical Structures, School of Aerospace, Xi’an Jiaotong University, Xi’an 710049, China School of Chemical Engineering, Northwest University, Xi’an 710069, China Earth Engineering Center, Center for Advanced Materials for Energy and Environment, Department of Earth and Environmental Engineering, Columbia University, New York, NY 10027, USA

Reversible CO2 capture from ambient air by a humidity swing has shown great potential in mitigating the greenhouse effect. In this work, we developed a new humidity-swing absorbent based on PO43-/HPO42-/H2PO4- ions exhibiting superior CO2 absorption capacity and kinetics compared to that of CO32-/HCO3--based absorbent. After ion exchange with PO43- ions, the ion-exchange resin (IER-PO4) containing positive quaternary ammonium groups and movable PO43- ions is able to reversibly capture CO2 from the ambient air by a humidity swing, which triggers the transformation between the PO43- ions and HPO42-/H2PO4- ions in the resin. In a dry environment, PO43- ions in IER-PO4 are hydrolyzed into OH- ions and HPO42- ions, which are further hydrolyzed into H2PO4- ions and OH- ions. Both hydrolysis reactions produce OH- ions for CO, absorption, while the adsorbed CO2 can be released in a humid environment. The results of quantum chemical calculation show that the hydrolysis of the ions is promoted by the reduction of water molecules in the nanoscale hydrated cluster. The adsorption capacity of IER-PO4 during the moisture swing is 80% larger than that of IER-CO3, and the adsorption rate of the IER-PO4 resin at a temperature range of 15-35 degrees C is much higher than that of the IER-CO3 absorbent. A modified pseudo-first-order (MPFO) kinetic is developed, which can describe the experimental results well. The present study sheds light on the design of high performance moisture-swing absorbents with PO43- ions.

基于硫酸根自由基(sulfate radical,SO4-·)氧化原理的活化过硫酸盐(persulfate,PS)氧化法是近年来高级氧化工艺(advanced oxidation process,AOP)的研究热点,以经济、高效、环境友好、安全稳定的优势在水处理、环境保护等领域开辟了新的思路.此前,学者们发现过硫酸盐高级氧化根据活化反应条件(如温度、光照、pH、过渡金属及催化剂等)的不同,会产生不同的自由基参与氧化反应,对降解结果也会产生不同程度的影响.本文根据相关自由基氧化机理,从产生硫酸根自由基的单一氧化、复杂活化体系硫酸根自由基与其他自由基复合氧化以及强化降解等方面,分析了近几年国内外学者对过硫酸盐降解典型有机污染物的研究及在催化剂开发方面所做的工作,指出了许多新颖的过硫酸盐活化手段及其降解效果与不足,并就未来的发展进行了展望,以期为过硫酸盐氧化法未来更好地发展和应用探索出路.

Although Cas9 nucleases are remarkably diverse in microorganisms, the range of genomic sequences targetable by a CRISPR/Cas9 system is restricted by the requirement of a short protospacer adjacent motif (PAM) at the target site. Here, we generate a group of chimeric Cas9 (cCas9) variants by replacing the key region in the PAM interaction (PI) domain of Staphylococcus aureus Cas9 (SaCas9) with the corresponding region in a panel of SaCas9 orthologs. By using a functional assay at target sites with different nucleotide recombinations at PAM position 3-6, we identify several cCas9 variants with expanded recognition capability at NNVRRN, NNVACT, NNVATG, NNVATT, NNVGCT, NNVGTG, and NNVGTT PAM sequences. In summary, we provide a panel of cCas9 variants accessible up to 1/4 of all the possible genomic targets in mammalian cells.

近年来,随着煤化工行业不断发展,废水排放量加大.煤化工行业废水排放量大、高盐和高化学需氧量的现状使得对其的处理成为一大热点和难点.本文以伊犁某工厂实际含盐有机废水(TDS含量25000mg/L)成分为依据,选取2-甲氧基苯酚作为煤化工废水中典型有机物,采用电化学协同过硫酸盐法处理含盐有机废水,主要考察电压、初始过硫酸钠浓度、极板间距及初始pH对2-甲氧基苯酚降解率的影响.结果表明,综合考虑电能消耗及氧化剂成本,在2V电压、极板间距3cm、过硫酸钠投加量5g/L、pH=12以及反应3h条件下,2-甲氧基苯酚的降解率可达到97.5％,相较单一的电化学法或过硫酸盐氧化法均有显著提升,协同效应明显.本文研究结果为今后煤化工行业含盐有机废水的绿色高效处理提供了一种新的思路.

In this paper,a multi-scale model combining the local transmembrane osmosis model and the mass transfer in flow channels in a full-scale pressure retarded osmosis(PRO)membrane module was set up to determine the performance of PRO in a full-scale operation(i.e.,power density and specific energy)by calculating the parameter distributions along feed and draw channels. This work focused on the effects of porosities,heights and numbers of layer of both feed and draw spacers on the performance of PRO. According to the numerical simulations,higher porosities of feed and draw spacer can achieve higher power densities but lower specific energy. Smaller height of feed spacer and larger height of draw spacer result in higher power densities while the specific energy increases as the heights of feed spacer and draw spacer decrease. Multilayer spacers were found to have adverse effects on the performance. Our findings give insight into designing membrane modules. Feed spacers should have relatively small porosity and small height while draw spacers can have relatively larger porosity and large height,and for both feed and draw spacers,monolayer spacers are recommended.

Through measurement of phase dimension via laser scattering, phase morphology development in immiscible blends of polyamide 12/poly(ethylene glycol) (PEG) with an extremely high viscosity ratio was investigated. The blends were prepared by melt blending in a batch mixer. The objective was to examine the influence of mixing time, rotor speed, as well as blending temperature on the size distribution of the minor phase. It is of interest that the breakup process of the dispersed PA 12 phase was observed for the blend systems even for extremely high viscosity ratios of <= 10(2)-10(3). Mixing time had a significant effect on the development of dispersed phase size distribution. It was found that the bulk of particle size reduction took place very early in the mixing process, and very small droplets with a diameter of 0.1-10 mu m were produced. The number of small particles then decreased, resulting in a larger average particle size. With further prolonged mixing, the particle size levels off. The particle size and its distribution were also found to be sensitive to the rotor speed. The average particle size decreased with increased rotor speed. The effect of blending temperature on size and size distribution, which has seldom been studied, was also examined in this work. When the blending temperature altered from 190 degrees C to 220 degrees C, the size and its distribution of the dispersed phase varied considerably, and the change of viscosity ratio was found to be the key factor affecting the dispersed phase size. (c) 2006 Wiley Periodicals, Inc.