ACS Nano
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2025
·
IF 16
Kang Lian,Sanshuang Gao,Wenxian Liu,Qian Liu,Yanhong Feng,Jun Luo,Guangzhi Hu,Ke Chu,Dingsheng Wang,Xijun Liu
The combination of CO2 fixation and small organic molecule oxidation offers a promising solution to increasing severe environmental issues and energy crises. Here, low-coordinated NiN3 sites were anchored onto nitrogen-doped ordered mesoporous carbon (Ni-SAs/NOMC), which is capable of efficiently catalyzing the coupled methanol oxidation reaction and CO2 reduction reaction (MOR||CO2RR), thereby reducing the energy required for CO2 conversion and enhancing the economic value of the CO2 electrolytic system. In the membrane electrode assembly electrolyzer-based MOR||CO2RR, Ni-SAs/NOMC achieved Faradaic efficiencies (FEs) of 95.4% for formate at the anode and 96.3% for CO at the cathode. Moreover, at a current density of 0.8 A cm–2, Ni-SAs/NOMC demonstrated stable electrolysis for up to 100 h, with FEs at both the anode and cathode remaining stable at approximately 90%. In situ spectroscopy analyses and theoretical calculations identified the formation of critical intermediate species and the origin of activity improvement, guiding the development of efficient electrosynthesis of valuable chemicals.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Shijie Yang,Guangbin Zhang,Zijie Lin,Zhihuan Li,Min Wang,Sheng Wang,Yuhui Sun,Zhongwei Yu,Pei Zhang,Linjiao Ren,Liying Jiang,Xiaoying Song,Yalong Zhao,Changshun Wang,Jing Wu,Linglong Zhang,Hucheng Song,Jun Xu
Lithium-carbon dioxide (Li-CO 2 ) batteries using high ion-conductive inorganic molten salt electrolytes have recently attracted much attention due to the high energy density and potential application of carbon neutrality. However, the poor Li-ion conductivity of the molten-salt electrolytes at room temperature (RT) makes these batteries lose most of their capacity and power as the temperature falls below 80 ℃. Here, inspired by the greenhouse effect, we report an RT molten salt Li-CO 2 battery where solar energy can be efficiently harvested and converted into heat that is further localized on the cathode consisting of plasmonic ruthenium (Ru) catalysts and Li 2 CO 3 -based products via a greenhouse-like phenomenon. As a result, the solar-driven molten salt Li-CO 2 battery demonstrates a larger full discharge/charge capacity of 9.5 mA h/8.1 mA h, and a longer cycle lifespan of 250 cycles at 500 mA/g with a limited capacity of 500 mA h/g at RT than the molten salt Li-CO 2 battery at 130 ℃. Notably, the average temperature of the cathode increases by 8 °C after discharge to 0.75 mA h, which indicates the infrared radiation from Ru catalysts can be effectively suppressed by discharged Li 2 CO 3 -based products. This battery technology paves the way for developing low-temperature molten salt energy storage devices.
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ACS Catalysis
·
2025
·
IF 13.1
Dongdong Chu,Mingkai Xu,Yunjie Zou,Chao Xing,Dayu Sun,Lan Ling
Hydrogen spillover has been widely recognized as a pivotal phenomenon in heterogeneous catalysis, yet the global impact of active hydrogen species on support materials remains underexplored, hindering the establishment of robust structure–performance correlations. In this study, we employed in situ scanning transmission electron microscopy (in situ STEM) to investigate the support effect in ruthenium-loaded molybdenum trioxide (Ru/MoO3) catalysts during the reversed water–gas shift reaction (RWGS). Our observations revealed that the presence of active hydrogen atoms markedly enhanced the evolution of lattice oxygen from MoO3, resulting in the transformation of the Ru-MoO3 nanosheet into a porous structure reminiscent of a jigsaw puzzle, thereby creating active CO2 sites on the catalytic surface. The controlled surface reconstruction of Ru-MoO3 enabled 14.3% CO2 conversion and nearly 100% CO selectivity at 300 °C, closely approaching the thermodynamic equilibrium limit of the RWGS reaction. These findings provide critical insights into the influence of active hydrogen on the morphology and crystal structure of supports at a comprehensive scale, underscoring its potential to enhance photothermal catalytic CO2 hydrogenation performance and paving the way for the development of more efficient CO2 conversion technologies.
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LANGMUIR
·
2025
·
IF 3.9
Hongbin Yang,Haocong Li,Haizhuang Jiang,Yubin Zhang,Luyao Xing,Xin Kang,Huazheng Wang,Shuhe Zhang,Haobin Shi,Wanli Kang
Nanopolymer microspheres have been widely studied in the development of low-permeability reservoirs as an effective material to improve foam stability. However, there are few studies on the foam stability mechanism of nanopolymer microspheres. In this work, the effect of surface hydrophobicity of fluorescent nanopolymer microspheres PARC(Flu-Ac) on the stability of CO2 foam was investigated by using foam performance as an evaluation index. The mechanism of foam stabilization by PARC(Flu-Ac) with different degrees of hydrophobicity was clarified by studying the drainage rate, micromorphology, interfacial rheology of foam, and adsorption behavior of microspheres on the foam liquid film. The results show that PARC(Flu-Ac)-5 microspheres with neutral wettability have the best foam stabilization effect. At 94 °C, the foam volume of CO2 foam is 630 mL and the foam half-life is 30.12 min. PARC(Flu-Ac)-5 microspheres have a high desorption energy and can stably adsorb at the gas–liquid interface to form a solid layer. The microspheres improve the mechanical strength of the foam and reduce the direct contact of the fluid, thus providing space resistance for thinning the liquid film and the diffusion of gas between bubbles. In addition, the microspheres can slow the thinning rate of the liquid film through the release of free water. The stability of the foam is significantly improved. This study further clarifies the enhancement mechanism of nanopolymer microspheres on the stability of CO2 foam, which has excellent guiding significance for the application of CO2 foam in low-permeability oil fields.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Jiang Yilin,Xi Ruonan,Yin Jinlin,Sun Chen,Li Yukong,Wu Chao,Zhang Chi,Fei Honghan
Three-dimensional lead halide hybrids exhibit excellent photophysical properties but suffer from inherent instability. In contrast, two-dimensional layered lead halides offer enhanced environmental stability, yet their strongly bound excitons restrict efficient charge transport. Here we present a covalent intercalation strategy involving the benchmark photosensitizer [Ru(bpy) 3 ] 2+ into a layered lead halide framework, featuring cationic [Pb 23 X 42 ] 4+ (X − = Cl − or Br − ) layers pillared by [Ru(bpy) 3 ] 2+ ligands via Pb 2+ -carboxylate coordination. This hybrid material achieves nearly full visible-light absorption and efficient photoinduced charge transfer from [Ru(bpy) 3 ] 2+ to the lead halide layers. This affords efficient CO 2 -to-CO photoreduction with an apparent quantum efficiency of ~3.0% at 500 nm, exceeding the performance of all previously reported organolead halide photocatalysts. Mechanistic studies indicate that the [Ru(bpy) 3 ] 2+ ligands enhance charge transport to Pb 2+ sites, facilitating CO 2 activation and reducing the reaction barrier for the *COOH intermediate. This work establishes a paradigm for intercalation chemistry in robust layered lead halide hybrids.
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MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Rumeng Gao,Lin Wang,Yayu Feng,Yunfei Liu,Lili Cao,Kuilin Deng
The red fluorescent polymers are indispensable but rare materials in the bio-imaging, probe and optoelectronic device fields due to the large penetration depth in tissues, high resistance to photobleaching, low toxicity and high luminescence efficiency. In this study, we designed an O/N/S-containing five-membered thiazolidinone as a “potential chromophore” to embed in macromolecular chains according to cluster-triggered emission (CTE). A series of polythiazolidinones (PTDs) were synthesized by one-step MALI polymerization using dialdehyde, diamine, and thioglycolic acid in the experiment. As expected, PTDs showed the enhanced red fluorescence emission at 600–620 nm with excitation-dependent fluorescence (EDF) due to the overlap of intramolecular and intermolecular electron clouds leading to the narrowed energy gap between the excited and ground states. Notably, PTD-A selectively recognized and detected Co 2+ ions even in the presence of 12 other metal ions and 10 anions with the detection limits of as low as 0.24 μM. Furthermore, the quenching mechanism of Co 2+ to PTD-A is attributed to static quenching caused by the coordination of Co 2+ ions with a coordination ratio of 1:1. In addition, the rapid on-site determination of Co 2+ in the real samples was achieved by the combination between PTD-A and smartphones without professional equipment. In brief, the successful preparation of polythiazolidinones provides a constructive reference for the molecular design of red light-emitting materials and their potential applications.
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Catalysts
·
2025
·Vol. 15
·期 11
·1037
·
IF 4
Ming Cai,Shaokun Lv,Yuanyuan Li,Wahyu Prasetyo Utomo,Yongsheng Yan,Zhi Zhu,Jun Zhao
Photocatalytic CO2reduction holds great potential for sustainable solar fuel production, yet its practical application is often limited by inefficient charge separation and poor product selectivity. The photothermal effect presents a viable strategy to address these challenges by reducing activation energies and accelerating reaction kinetics. In this work, we report a rationally designed CN-B/Ti3C2heterojunction that effectively leverages photothermal promotion for enhanced CO2reduction. The black carbon nitride (CN-B) framework, synthesized via a one-step calcination of urea and Phloxine B, exhibits outstanding photothermal conversion, reaching 131.4 °C under 300 mW cm−2illumination, which facilitates CO2adsorption and charge separation. Coupled with Ti3C2MXene, the optimized composite (3:1) achieves remarkable CO and CH4production rates of 80.21 and 35.13 μmol g−1h−1, respectively, without any cocatalyst—representing a 2.9-fold and 8.8-fold enhancement over CN-B and g-C3N4in CO yield. Mechanistic studies reveal that the improved performance stems from synergistic effects: a built-in electric field prolongs charge carrier lifetime (3.15 ns) and reduces interfacial resistance, while localized heating under full-spectrum light further promotes CO2activation. In situ Fourier transform infrared (FTIR) spectroscopy confirms the accelerated formation of key intermediates (*COOH and *CO). The catalyst also maintains excellent stability over 24 h. This study demonstrates the promise of combining photothermal effects with heterojunction engineering for efficient and durable CO2photoreduction.
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Advanced Science
·
2022
·Vol. 9
·期 16
·2105292
·
IF 17.521
Yawen Jiang,Xinyu Wang,Delong Duan,Chaohua He,Jun Ma,Wenqing Zhang,Hengjie Liu,Ran Long,Zibiao Li,Tingting Kong,Xian Jun Loh,Li Song,Enyi Ye,Yujie Xiong
Structural reconstruction is a process commonly observed for Cu-based catalysts in electrochemical CO 2 reduction. The Cu-based precatalysts with structural complexity often undergo sophisticated structural reconstruction processes, which may offer opportunities for enhancing the electrosynthesis of multicarbon products (C 2+ products) but remain largely uncertain due to various new structural features possibly arising during the processes. In this work, the Cu 2 O superparticles with an assembly structure are demonstrated to undergo complicated structure evolution under electrochemical reduction condition, enabling highly selective CO 2 -to-C 2+ products conversion in electrocatalysis. As revealed by electron microscopic characterization together with in situ X-ray absorption spectroscopy and Raman spectroscopy, the building blocks inside the superparticle fuse to generate numerous grain boundaries while those in the outer shell detach to form nanogap structures that can efficiently confine OH − to induce high local pH. Such a combination of unique structural features with local reaction environment offers two important factors for facilitating C−C coupling. Consequently, the Cu 2 O superparticle-derived catalyst achieves high faradaic efficiencies of 53.2% for C 2 H 4 and 74.2% for C 2+ products, surpassing the performance of geometrically simpler Cu 2 O cube-derived catalyst and most reported Cu electrocatalysts under comparable conditions. This work provides insights for rationally designing highly selective CO 2 reduction electrocatalysts by controlling structural reconstruction.
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CARBOHYDRATE POLYMERS
·
2024
·
IF 10.7
Feilin Lin,Jianzhong Jiang
Emulsions have extensive applications in food, cosmetics, and agriculture, while the requirements for emulsions differ in various fields. It is a challenge for one emulsion to satisfy multiple requirements in different applications. Herein, CO 2 -switchable emulsions with controllable stability and viscosity were prepared by a mixture of chitosans (CS) and CTAB. After adding low concentrations of CTAB (e.g. 0.5 mM), the viscous Pickering emulsions stabilized by CS alone were converted into moderate-viscous Pickering emulsions due to the competition adsorption between CS aggregates and CTAB at the oil-water interface. The transformation of emulsion types (such as Pickering and conventional emulsions) and the emulsion's stability and viscosity were controlled by CO 2 /N 2 trigger. Furthermore, at high CTAB concentrations (≥ 0.8 mM), a novel long-term stable conventional emulsion was obtained after the CS aggregates at the oil-water interface were entirely replaced by CTAB. Compared with other stimuli, CO 2 is recognized as a green trigger that doesn't cause contaminations in the system, which has potential applications in organic synthesis and polymerization. Our strategy provides a simple and effective method to smartly control the properties of the emulsions (such as the emulsion type, stability, and viscosity), obtaining an intelligent emulsion to meet different requirements in many applications.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ming-Long Wang,Yi-Fei Sun,Hong-Nan Chen,Jin-Rong Zhong,Dan Rao,Yu Liu,De-Jun Xuan,Bei Liu,Chang-Yu Sun,Guang-Jin Chen
The CO 2 -H 2 O emulsion has multiple advantages in forming hydrate, such as easily adjustable CO 2 -to-H 2 O ratio, large contact area, strong sweep efficiency, and ability to carry chemical agents, which holds great promise for large-scale solid CO 2 geological sequestration. This paper systematically investigates the kinetics of hydrate formation from CO 2 -H 2 O emulsion and the corresponding morphological features in glass beads under different pore sizes at 3.27–7.15 °C and 10–14 MPa. Quantitative results on CO 2 hydrate formation rates, quantities, conversion rates, and hydrate saturations are obtained. Overall, under multi-factors, the conversion rates of CO 2 hydrate range from 22.9 % to 56.3 %, and hydrate saturations range from 18.5 % to 45.4 %. Here, lower temperature and higher pressure can enhance hydrate formation and increase the final conversion rate. As the pore size decreases, CO 2 hydrate conversion ratio increases, but the formation rate shows a significant decline. Additionally, under flowing conditions, hydrate conversion rates are further increased to 44.4 %–76.5 %, and its enhancement mechanism has been observed and revealed. Even though CO 2 droplets remain spatially separated, hydrate formation still demonstrates remarkably rapid propagation. These results prove the potential of CO 2 emulsion as an excellent medium for CO 2 hydrate storage and provide a direction for more effective carbon storage.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Ruiqi Zhang,Yanyan Zhang,Kang Wang,Xitao Wang,Baoquan Zhang
In this work, the heterostructure between Cu particles and ZnFe-LDH semiconductor with lantern shape was constructed by reducing the ternary CuZnFe-LDH using H 2 , and the effects of Cu loading and the formation of heterojunction on photocatalytic CO 2 reduction to CO and CH 4 were investigated. The results showed that the hollow and layer-stacking structure of the catalyst was beneficial to the light utilization, adsorbing and activating of carbon dioxide. The Cu cations could enter into the lattice of ZnFe-LDH to form a ternary CuZnFe-LDH, which could be reduced to Cu particles with smaller size by H 2 and resulting in the heterostructure between Cu and ZnFe-LDH. The loading of Cu particles can significantly enhance the light absorption, photogenerated carriers transfer rate and separation efficiency of ZnFe-LDH, thus improving photocatalytic activity. As expected, Cu 1.6 ZnFe-R catalyst exhibited the highest catalytic activity with CO yield of 45.35 μmol·g cat −1 ·h −1 and CH 4 yield of 39.33 μmol·g cat −1 ·h −1 , which were 2.81 and 6.19 times higher than those of ZnFe-LDH, respectively. Meanwhile, Cu particles acted as electron-rich centers and CO 2 adsorption sites can noticeably improve the CH 4 selectivity and inhibit H 2 production. The Cu 1.6 ZnFe-R catalyst exhibits the highest CH 4 electron-based selectivity of 65.17 %, the highest electrons consumed of 482.80 μmoL·g cat −1 ·h −1 for CO 2 reduction and the lowest H 2 electron-based selectivity of 16.04 %.
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Small
·
2025
·
IF 12.1
Yu-Ren Xue,Guang-Chang Xu,Kai Li,Xin-Yu Guo,Jian Wu,Hong-Qing Liang,Hao-Cheng Yang,Chao Zhang,Zhi-Kang Xu
The growing demand for energy-efficient carbon capture has spurred significant advancements in supported ionic liquid membranes (SILMs), which utilize ionic liquid (IL) with high CO 2 solubility for continuous gas purification processes. However, conventional SILMs are hindered by a persistent limitation: thick IL layers (> 50 µm) significantly reduce CO 2 permeance to below 1 GPU, while also causing mechanical failure under prolonged operational pressure. Inspired by the interlocking elytra of Tenebrionidae beetles, which use microscale “teeth” to withstand mechanical stress, locked ionic liquid membranes (LILMs) are engineered by composeing two interpenetrating polyamide nanofilms with biomimetic protrusions. These nanofilms confine ILs within cavities formed by protrusions, thinning IL layers to sub-0.5 µm while resisting shear stresses. The LILMs demonstrate a CO 2 /N 2 selectivity of 55 and an enhanced CO 2 permeance of 8.2 GPU, surpassing the performance of conventional SILMs by ≈20-fold while maintaining stability over 168 h of continuous mixed gas separation. By dual-purposing ILs as both solvents for interfacial polymerization and CO 2 transporters, this bio-inspired architecture overcomes the thickness-stability limitations, enabling energy-efficient carbon capture.
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