Nature Communications
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2025
·Vol. 16
·期 1
·10497
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IF 15.7
Wang Zhijie,Zhou Yimian,Ni Wenkang,Li Jianfei,Yue Xuanyu,Zhang Zizhong,Dai Wenxin,Fu Xianzhi
Cu-based nanocatalysts hold promise for the reverse water–gas shift (RWGS) reaction. However, irreversible sintering of the Cu catalyst for deactivation remains a persistent challenge under thermal or photothermal processes. In this study, we develop an anti-sintering catalyst using CuNiMgAl layered-double-hydroxide (LDH)-derived hydroxyl engineering to anchor ultrafine CuNi nanoparticles, achieving stable photothermal RWGS conversion. For Cu 3 Ni-MA, the oxyphilic Ni dopants facilitate the formation of hydroxyl-coordinated Cu 2+ –Ni 2+ species during the calcination of LDH-derived materials; meanwhile, the Ni incorporation enhances the plasmonic effect of CuNi nanocatalysts to drive H 2 spillover for hydroxyl replenishment under light irradiation, which is diverged from conventional Cu 3 Ni alloy-based catalysts. This Cu 3 Ni-MA achieves a CO production rate of 339.8 mmol g −1 h −1 with 98% selectivity, outperforming thermal catalysis by 3.5-fold in RWGS conversion. Notably, the catalyst exhibits robust photothermal CO 2 hydrogenation stability, preserving >99% of its original activity and CO selectivity during 30 d of intermittent start–stop cycles and 280-h continuous testing. This study offers alternative perspectives for designing anti-sintering catalysts for photothermal catalytic systems by coupling dynamic hydroxyl regulation with plasmonic activation mechanisms.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yanni Ran,Kang Peng,Ziyan Li,Xingwang Guo,Honglin Chen,Shengxuan Cai,Lei Su,Min Niu,De Lu,Hongjie Wang
CO 2 capture can mitigate carbon emissions with the objective of achieving carbon neutrality. Solid amine adsorbents have emerged as one of the most promising materials for capturing CO 2 . However, balancing the diffusion and adsorption of CO 2 remains a significant challenge, making it difficult to achieve high capacity and rapid kinetics simultaneously. In this study, SiC nanowires aerogel (SiCNWA) was functionalized with tetraethylenepentamine (TEPA) and diethanolamine (DEA) for CO 2 capture. The optimal adsorbent was synthesized with a total amine loading of 90 wt%, comprising 75 wt% TEPA and 25 wt% DEA. It exhibits a high CO 2 adsorption capacity of 4.71 mmol/g and ultra-rapid adsorption kinetics, achieving 80 % adsorption capacity within the first minute. The advantageous properties stem from the synergistic effects arising from the unique three-dimensional network structure of SiCNWA, coupled with the complementary group interactions of the hybrid amines. The ultra-high porosity of aerogel facilitates a high proportion of amine loading and dispersion, contributing to its high CO 2 adsorption capacity. Additionally, the continuous network structure offers efficient channels for CO 2 transport, enabling ultra-rapid CO 2 adsorption kinetics. The high amine density of TEPA provides abundant adsorption sites for CO 2 , and the addition of DEA can effectively mitigate the aggregation and deactivation of amine groups, thereby significantly improving the adsorption rate and adsorption capacity. This aerogel-hybrid amines strategy effectively balances diffusion and adsorption, offering valuable insights for advancing aerogel-based materials for CO 2 capture.
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CERAMICS INTERNATIONAL
·
2025
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IF 5.6
Yan Lin,Min Xu,Xi Chen,Sixie Chen,Xiang Li,Wenle Yan,Ruixue Zhou,Di Chen
Solid oxide electrolysis cells (SOECs) are promising energy conversion devices capable of efficiently converting CO 2 into valuable products taken the advantage of heat and renewable electricity sources. The performance of SOECs is largely influenced by the cathode material, which governs the electrochemical reduction of CO 2 . In this work, we engineered metal-perovskite cathode by pre-depositing Cu nanocrystal onto the surface of La 0.1 Ca 0.9 Fe 0.1 Ti 0.9 O 3-δ (LCFT) cathode to well understand the effects of Cu metal nanocrystal in high temperature CO 2 reduction. This Cu nanocrystal deposition on cathode resulted in a significant reduction in polarisation resistance of SOEC by 50 % improved current density from 310 mA cm −2 to 456 mA cm −2 at 1.6 V. The cell also exhibits good stability over 100 h without obvious degradation. Extensive structural and chemical analyses indicate the deposited Cu nanocrystal facilitated the formation of oxygen vacancies and metal-oxide interface which should attribute to the enhanced electrochemical performance. This study provides new insights into the role of metal decoration in facilitating the high temperature direct CO 2 electrolysis performance.
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ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Ruifang Zhang,Dekai Liu,Lei Mao,Guangzhang Liu,Yanhong Zhou,Yaxin Chen,Chun Yang,Zicheng Wu,Wei Jiang,Guangya Zhang
Carbonic anhydrase (CA) had immense potentials in addressing the escalating atmospheric carbon dioxide (CO2) levels; however, it was hindered by poor stability, high purification costs, and difficult recycling. A novel one-pot polydopamine (PDA)–Fe2+ coating strategy was proposed to immobilize “mega-CA”, namely, the nanosized SazCA-ferritin assemblies (nsSazCA-F) with an exceptionally large size (21 nm × 21 nm × 21 nm) and ultrahigh molecular weight (1224 kDa). Leveraging low-concentration Fe2+ to accelerate dopamine polymerization on porous nickel foam (NF), a hierarchically porous PDA-Fe2+-nsSazCA-F@NF coating was fabricated within 20 min, demonstrating 82.5% activity retention after 10 reuse cycles and a significantly extended half-life of 70.7 ± 3.9 days (55% improvement compared to free enzymes) at 30 °C and pH 8.0. Furthermore, an integrated PDA-Fe2+-nsSazCA-F@NF coating–Chlorella system was developed for direct air CO2 capture, achieving a 58% increase in Chlorella biomass and a 60% enhancement in the CO2 fixation rate over 8 days, which offered a novel paradigm for achieving air carbon neutrality. The proposed strategy presents a promising approach for efficient immobilization of “mega-enzymes”, providing a new solution for clean production and sustainable carbon cycling technologies.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Jingce Bi,Nianzhu Yang,Huichun Xue,Ningning Liu,Yi Wang,Xia Zhang,Zhuopeng Wang,Lin Zhu,Yide Han
Molten salt-assisted pyrolysis has emerged as an effective strategy for engineering defective/doped g-C 3 N 4 photocatalysts for CO 2 reduction. While K + incorporation enhances interlayer charge transport, excessive K + generates detrimental nitrogen vacancies that destabilize the heptazine framework and compromise carrier mobility. Herein, we developed S/K co-doped graphitic carbon nitride (g-C 3 N 4 ) with tunable nitrogen vacancies (denoted SWCN-M) via molten salt (KCl-LiCl) pyrolysis of sulfur-containing supramolecular precursors (melamine with thiourea or thioacetamide). The nitrogen vacancy concentration is precisely modulated by the choice of sulfur precursor (thiourea vs. thioacetamide) to optimize the synergy effect of K + -N-vacancy, and eventually boosting photocatalytic performance. The thiourea-derived SWCN-M TU achieves a CO evolution rate of 165.7 μmol g −1 h −1 , outperforming its thioacetamide analogue (SWCN-M TAA , 90.4 μmol g −1 h −1 ), pristine WCN (53.8 μmol g −1 h −1 ), and K-doped WCN-M (64.3 μmol g −1 h −1 ) by factors of 1.8, 3.1, and 2.6, respectively. DFT calculation results reveal that S-doping induces charge localization, elevating the N-vacancy formation energy via Coulombic repulsion with K + . This work advances the rational design of vacancy-engineered carbon nitride for photocatalytic CO 2 reduction
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LANGMUIR
·
2025
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IF 3.9
Chenxiang Feng,Wei Jian,Junxiu Chen,Agula Bao
The environmental problems caused by excessive CO2 emissions have made the development of adsorbent materials for capturing CO2 an important topic. N-doped porous carbon materials are attractive for CO2 adsorption because of their large specific surface area, porous structure, and multiple active sites. S and N are known to work well together as codopants, but the effects of S on N and the synergistic effects of S and N on carbon materials need to be clarified. In this study, N and S codoped porous carbon samples with an ultramicroporous structure were prepared by using lignin as the carbon source and thiourea as the sulfur source. The prepared samples had a specific surface area of up to 1723 m2/g and N and S contents of up to 1.60 at % and 0.23 at %, respectively. In tests, the best-performing sample had a CO2 adsorption capacity of 3.58 mmol/g at 298 K and 1 bar, which can be attributed to ultramicropores (<1 nm) making up 67.8% of the pore volume. S doping had the synergistic effect of increasing the pyrrole N content on the sample surface, which increased the CO2 adsorption capacity. The present study provides insights into using N and S codoping to develop high-efficiency carbon-based adsorbents for CO2 capture.
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ACS Applied Polymer Materials
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2025
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IF 4.7
Jun Cai,Yang Song,Yunfei Yu,Jie Chen,Chao Wang,Xiaoli Ding,Xue Yang,Jianqiang Meng
Ion gel membranes exhibit high efficiency and environmental friendliness for CO2/N2 separation, but their poor mechanical strength and inability to self-heal after physical damage hinder their industrial application. To overcome these limitations, we propose an efficient one-pot method for preparing dual-network (DN) ion gel membranes with enhanced gas separation and self-healing properties. This method involves constructing dual self-healing networks: the first network (FN), formed through a Schiff base reaction between O,O’-bis(2-aminopropyl)poly(propylene glycol)-block-poly(ethylene glycol)-block-poly(propylene glycol) (H2N–PPG-PEG-PPG-NH2) and 1,3,5-benzenetricarboxaldehyde (BTC), and the second network (SN), consisting of polyurethane (PU) featuring a quadruple hydrogen-bonded cross-linked network. By optimizing the ratio of the two networks to 5:2 and adjusting the ionic liquid content ([EMIM]TFSI) to 60 wt %, the resulting DN membrane demonstrates exceptional CO2 gas separation performance, with a CO2 permeability (PCO2) of 726 Barrer and a selectivity (αCO2/N2) of 23. This underscores the potential of this process for effective gas separation applications. Furthermore, compared to conventional ion gel membranes, the DN membranes exhibit significant improvements in mechanical properties and self-healing capabilities, while maintaining high CO2 permeability and selectivity.
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BIORESOURCE TECHNOLOGY
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2025
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IF 9
Ruixue Ma,Jun Cheng,Ying Liu,Dongwei Jia,Jiahao Wang
Given that excessive CO 2 induces reactive oxygen species (ROS) which inhibit photosynthesis and microalgal survival, this study explores how exogenous arginine enhances stress resilience and biomass yield of Nannochloropsis oceanica under high CO 2 stress. Arginine promoted NO synthesis, enhancing antioxidant enzyme activities to combat ROS damage. Transcriptomic analysis revealed that key enzymes in the Calvin cycle (PRK, GAPDH, FBPase and SBPase) and TCA cycle (CS, IDH, SCS and MDH) were significantly up-regulated, supporting carbon fixation and energy metabolism. Arginine also alleviated cell necrosis by extending the G1 phase, promoting DNA replication and protein synthesis, which increased the proportion of viable cells from 47 % to 84 %. Furthermore, the synthesis of chlorophyll a and carotenoid were enhanced, leading to 46 % increase in biomass yield. The results highlighted arginine as a promising metabolic regulator for enhancing stress tolerance and carbon fixation efficiency of N. oceanica under high CO 2 conditions.
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Small
·
2025
·
IF 12.1
Deguang Ji,Zi Yang,Yaxiong Yao,Yichao Hou,Zidong He,Pengfei Da,Wei Shen,Li An,Yuanmiao Sun,Pinxian Xi,Chun-Hua Yan
Copper-based catalysts show considerable promise in the electrochemical CO 2 reduction reaction (CO 2 RR) for the production of hydrocarbons and oxygenates, particularly methane (CH 4 ), which is a highly reduced product. The high-valent state of copper (Cu) exerts a positive influence on the formation pathway of CH 4 , but the reduction potential will lead to a decrease in the valence state during CO 2 RR. In this study, a highly crystalline and structurally well-defined Y 2 Cu 2 O 5 catalyst is constructed to stabilize Cu 2+ with the orderly alternating Y─O skeleton layer, owing to the strong bonding interaction. The Y 2 Cu 2 O 5 exhibits a remarkable enhancement in CH 4 selectivity compared to CuO (up to 9.59-folds), achieving a selectivity of 61.3% at 300 mA cm −2 and 58.4% at 400 mA cm −2 , together with good stability. In situ attenuated total reflectance Fourier transform infrared spectra (ATR-FTIR) and density functional theory (DFT) calculations reveal that the presence of the Y─O skeleton layer in Y 2 Cu 2 O 5 significantly enhances the adsorption of *CO intermediate, and accelerates its hydrogenation process, facilitating the conversion of CO 2 to CH 4 . This work highlights Y─O skeleton-mediated stabilization of Cu 2+ for efficient electroreduction of CO 2 to CH 4 , providing valuable insights into the design of efficient electrocatalysts for CO 2 conversion.
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Materials
·
2025
·Vol. 18
·期 6
·1343
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IF 3.2
Hangmin Xu,Hao Song,Xiaozhi Wang,Xingwang Zhu
The substantial release of industrial carbon dioxide has been identified as a key factor in the development of various environmental issues. In addressing these concerns, the utilization of photocatalytic technology for carbon reduction has garnered significant attention. The disadvantage of CO2photoreduction is the problem of product yield and selectivity. It is known that MIL-125(Ti) with a high specific surface area (SBET) possesses more active sites using Ti as a node. The calcination of MIL-125(Ti) in a reducing atmosphere has been shown to introduce oxygen vacancies (OV), thereby enhancing the material’s surface and internal pores. This process has been demonstrated to result in a significant increase in the SBETand an enhancement of the Ti3+/Ti4+ratio. The increased Ti3+centers have been found to improve the material’s reducing properties. The results demonstrate that the OV-rich MIL-125-2H material exhibits the high-performance and highly selective photoreduction in CO2.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
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IF 3.5
Hu Yaping,Zhai Shasha,Guo Yaping,Dang Shan,Li Jing,Yang Miao
Electrochemical reduction reaction of CO 2 (CO 2 RR) to C 1 and C 2 products can be achieved on Cu-based electrocatalysts. C 2 products exhibit higher energy density and economic value compared to C 1 products, making them more desirable as reduction products. However, the production of C 2 products on pure Cu catalysts involves multi-step proton-coupled electron transfer and C–C coupling steps, which are kinetically slow and result in poor catalytic activity and selectivity for the products. The cavity nanocubes Cu 2 O(0.13-AA), Cu 2 O(0.10-AA) and Cu 2 O(0.15-AA) catalysts were synthesized via wet chemical reduction by adjusting the concentration of the reducing agent. The electrochemical pre-reduction method was used to obtain Cu 2 O/Cu(0.13-AA), Cu 2 O/Cu(0.10-AA) and Cu 2 O/Cu(0.15-AA) catalysts for CO 2 RR. Cu 2 O/Cu(0.13 M-AA) catalyst achieves the high Faradaic efficiency (FE) of 39.98% for C 2 H 4 and 54.76% for C 2 products (C 2 H 4 , C 2 H 6 , and C 2 H 5 OH), with significant inhibition of the hydrogen evolution reaction. In situ Raman experiments demonstrate that the cavity structure of the nanocubes enhances the local concentration of *CO intermediates, thereby promoting the C–C coupling process and improving the selectivity of CO 2 reduction to C 2 products.
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Molecular Catalysis
·
2024
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IF 3.9
Pinfang Yan,Xinyu Li,Jilei Wang,Jiahang Pan,Hu Xu,Yinhua Zhu,Qiaoling Chen,Hua Mei,Yan Xu
The design of efficient and low-price photocatalysts is an effective way to relieve excessive carbon dioxide emissions and energy dilemma. Polyoxometalates are ideal materials due to their adjustable structures and semiconductor-like properties. Limited by their light absorption capacity, it is a feasible way to construct inorganic-organic composite polyoxometalate-based photocatalysts. Here, two efficient Anderson-type polyoxometalate-based photocatalysts, (C 10 H 9 N 2 )·{[Co(H 2 O) 2 ]·[H 6 CrMo 6 O 24 ]}·4H 2 O ( 1 ), {[Co(H 2 O) 3 ]·[Co(DAPSC)] 2 ·[H 6 CrMo 6 O 24 ] 2 }·11H 2 O ( 2 ) [2,6-diacetylpyridine bis(semicarbazone), abbr. DAPSC], were prepared by hydrothermal synthesis method. The structural analysis indicates that compounds 1 and 2 share similarities: {CrMo 6 } units were linked by cobalt ions to form two-dimensional (2D) frameworks. The addition of Co ions provided catalytic active center for the catalyst, compounds 1 and 2 exhibited promising yield into CO, as high as 3061.6 μ mol g −1 ·h −1 and 9309.8 μ mol g −1 ·h −1 , respectively. Due to their excellent properties, Anderson-type POMs can be used as the basic units of photocatalysts. At the same time, four cycling tests prove the stability of compound 2 under a long reaction time.
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