Journal of Energy Chemistry
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2025
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IF 14.9
Chaoran Yang,Shuyu Liang,Cong Zhang,Tianyu Zhang,Wenfu Xie,Min Li,Qiang Wang
Copper (Cu)-based catalysts have demonstrated promising selectivity and activity in electroreducing CO 2 to multi-carbon (C 2+ ) products. Among them, oxide-derived Cu catalysts exhibit high selectivity for C 2+ products in the CO 2 electroreduction reaction (CO 2 RR). Cu chalcogenide-derived catalysts offer a promising approach to tune the electronic structure of Cu sites via surface reconstruction, thereby affecting the product distribution. However, the effect of in-situ anion dissolution, especially Se ions, on the electronic structure of Cu selenides at negative potentials remains overlooked, despite its potential to significantly affect catalytic activity. In this study, we developed a series of Cu selenide catalysts with varying Cu/Se ratios to optimize electronic structures and enhance CO 2 RR performance. Among them, Cu 1.8 Se, featuring Cu vacancies, exhibited the highest activity for C 2+ products formation and the highest C 2+ /C 1 products ratio, nearly 2–3 times greater than the others. This catalyst also demonstrated good stability over 38 h of electrolysis under −450 mA cm −2 , with a maximum C 2+ products Faradaic efficiency (FE) of up to 70 %. In-situ surface reconstruction analysis revealed Se loss and Cu + /Cu 2+ reduction of the initial Cu 1.8 Se catalyst, forming Cu/Cu x Se structures with Cu vacancies, identified as the real active sites. Density functional theory (DFT) calculations and in-situ infrared absorption spectroscopy confirmed that Cu vacancies play a critical role in stabilizing *CHOCO intermediates for C–C coupling while suppressing hydrogen evolution reaction and C 1 products formation. These findings highlight Cu vacancy engineering as an effective strategy for enhancing C 2+ selectivity in CO 2 RR.
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Sustainable Materials and Technologies
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2025
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IF 9.2
Shiyu Huang,Deqi Fan,Chengxiao Zhao,Xin Li,Xiaofei Yang
The photocatalytic conversion of anthropogenic carbon dioxide (CO 2 ) into solar fuels using semiconductor nanomaterials represents a promising and sustainable approach to addressing both energy sustainability and climate change concerns. Developing highly efficient semiconductor-based photocatalysts to tailor reaction pathways of CO 2 reduction is the key to producing value-added products with desirable performance. Herein, we report a novel copper-doped indium oxide (Cu-doped In 2 O 3 ) nanostructure prepared via the electrospinning technique, followed by annealing to enhance photocatalytic CO 2 reduction. Our findings demonstrate that modifying the bulk In 2 O 3 with copper enables Cu-doped In 2 O 3 nanofibers to catalyze the CO 2 reduction reaction more efficiently. In situ FTIR spectra measurements were utilized to identify the reaction intermediates and gaseous products for validating the reaction pathway. Combined with in situ electron paramagnetic resonance (EPR) and vibrational spectroscopy measurements, which revealed that interstitial Cu doping induces lattice distortions and oxygen vacancy (O V ) formation, effectively enhancing visible light absorption, accelerating charge separation, and migration. Consequently, the optimized In 2 O 3 -Cu3% nanofiber photocatalyst demonstrated outstanding selectivity (100 %) and a CO production rate of 45.5 μmol·g −1 ·h −1 , which is approximately six times higher than In 2 O 3 . Mechanistic studies have indicated that O V defects serve as electron reservoirs to suppress the recombination of photogenerated charges, while simultaneously creating abundant CO 2 chemisorption sites in nanostructures.
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JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Weihao Liu,Xu Jiang,Yan Yang,Lei Guo,Haoyang Wang,Lu Shao
Constructing high-performance mixed matrix membranes (MMMs) with highly permeable polymers of intrinsic microporosity (PIMs) and metal-organic frameworks (MOFs) faces critical challenge of poor interfacial compatibility between MOF fillers and the polymer matrix and difficulty in maintaining a defect-free interface at high filler loading (over 30 %). In this study, a Bi-HHTP loading as high as 50 wt% and uniform dispersion with excellent interfacial integrity is achieved in our high-performance MMMs through the elaborate design of multiple synergistic interfacial interactions, including hydrogen bonding between the phenolic hydroxyl groups of the 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) ligand in the Bi-HHTP filler and the cyano groups in the PIM-1 matrix and π-π stacking between their benzene ring structures. The optimized MMM exhibits a remarkable CO 2 permeability up to 4021 Barrer with an ideal CO 2 /N 2 selectivity of 42.1 which substantially outperforms the neat PIM-1 membrane and exceeds the 2019 upper bound. The enhanced separation performance of the MMMs stems mainly from the significant increase in CO 2 solubility selectivity with Bi-HHTP loading, which benefits from the inherent CO 2 affinity of Bi-HHTP and the effective suppression of N 2 dissolution by the rigidification of PIM-1 chain segments induced by strong interfacial interactions. Most importantly, the resulted high-loading MMMs exhibited remarkable structural stability, showing strong resistance to both physical aging and CO 2 -induced plasticization. This strategy overcomes the loading bottlenecks of state-of-the-art MMMs and contributes advanced membrane materials for efficient CO 2 capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Mian Zhu,Chao Lyu,Feng Dai,Jingxian Liu
To develop an environmentally friendly CO 2 capture technology, composite adsorbent beads were synthesized through the in situ growth of ZIF-8 in a nanocellulose gel scaffold prepared from pine needles-derived cellulose. The composite beads were subsequently functionalized with three ionic liquids ([BMIM][PF 6 ], [BMIM][BF 4 ], and [EMIM][TF 2 N]), which induced partial dissolution of the nanocellulose. This process resulted in the formation of unique wrinkled microstructures, resembling rice grains in morphology but exhibiting higher compressive strength. Notably, the IL-loaded CNF/ILs@ZIF-8 composites exhibited significantly superior adsorption performance over unmodified CNF@ZIF-8 (CZ) beads. Under static conditions (3 bar, 273 K), all three functionalized CNF/ILs@ZIF-8 variants enhanced CO 2 uptake capacities by > 46 %, with the [BMIM][PF 6 ] modified beads retaining 85.36 % of initial adsorption capacity after six adsorption–desorption cycles. Furthermore, under competitive dynamic adsorption (1 bar, 273 K), the [BMIM][BF 4 ] modified beads achieved a 43.12 % enhancement in CO 2 /N 2 selectivity compared to CZ. This work provides a MOF granulation strategy with process safety and environmental sustainability, potentially extending MOF applications in gas adsorption technologies.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yulan Xu,Minxian Wu,Xianxian Zhang,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Electrodeposition is a simple and rapid method for the preparation of thin-film materials, allowing catalytic materials to be directly deposited onto substrates, thereby eliminating the need for binders. Compared with bulk materials, two-dimensional thin films possess a higher specific surface area. The incorporation of Ga in Sn-based alloy materials can effectively expose active sites, thereby enhancing the catalytic performance for CO 2 electroreduction. Doping with rare-earth elements such as cerium can induce the formation of oxygen vacancies and defect sites, or modulate the electronic structure of the catalyst surface. These modifications enable independent regulation of the adsorption energy of various intermediates, effectively lowering reaction energy barriers and improving catalytic efficiency. In this work, Ga-Sn-Ce electrodes were synthesized via electrodeposition in a deep eutectic solvent composed of choline chloride and urea, and subsequently applied to CO 2 reduction. The GaSnCe0.6 electrode exhibited excellent selectivity toward formic acid at −0.99 V vs. the reversible hydrogen electrode, achieving a Faradaic efficiency of 92 %. Compared with previously reported Ga-Sn alloys, the introduction of Ce resulted in a positive shift of 250–270 mV in the optimal reduction potential for formic acid production from CO 2 .
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MOLECULES
·
2025
·Vol. 30
·期 17
·3475
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IF 4.6
Xiaoqian Xu,Song Yang,Yixiang Wang,Ying Chen,Assa Aravindh Sasikala Devi,Feng Hu
Silver is a promising electrocatalyst for electrochemical CO2reduction reaction owing to its high selectivity and efficiency for CO production. However, it still faces a fundamental trade-off between reaction activity and stability. Here, we developed a three-dimensional coral-like porous silver (CP-Ag) catalyst through seed-assisted nanoparticle attachment synthesis, which creates a unique architecture featuring interconnected pores and stable grain boundaries (GBs) between constituent Ag nanoparticles (Ag NPs). Compared to normal Ag NPs, CP-Ag demonstrates superior catalytic performance, maintaining >90% Faradaic efficiency (FE) for CO across a wide potential range (−0.6 to −1.0 V vs. RHE) while achieving 2-times higher current density. Importantly, CP-Ag demonstrated an impressive long-term stability by sustaining nearly 90% FE for CO approximately 40 h at a current density of −50 mA cm−2in a flow cell. The enhanced catalytic performance arises from three factors: (1) the three-dimensional coral-like morphology increases accessible active sites and promotes charge transfer efficiency; (2) stable GBs between interconnected nanoparticles increase reaction activity; (3) more moderate binding on Ag (100) preferentially promotes *CO intermediate formation. Our findings highlight the importance of simultaneously engineering both morphological and crystallographic features to optimize silver catalysts for CO2conversion.
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ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Mingxiu Lv,Hao-Nan Li,Jia-Hui Xin,Guang-Chang Xu,Shuhui Ma,Chuang-Wei Gu,Zhanbo Li,Zherui Chen,Chao Zhang,Yajun Deng,Xiao-Jun Huang,Zhi-Kang Xu
Ionic liquids (ILs) featuring excellent selective solubility for CO 2 have led to versatile development and applications of gas separation membranes for CO 2 capture. Over the past decade, a myriad of ILs-based membranes have been exploited; however, they normally suffer from a formidable conflict between CO 2 permeance and stability as imposed by their mutually exclusive design requirements. Herein, a photothermal-steered confined gelation and locking engineering (CGLE) is proposed to fabricate ultrathin dual-confined ionogel membranes (DCIMs) that empower ultrapermeable and durable CO 2 separation. In the CGLE, coupling CNTs-enabled photothermally confined reactor with ILs-regulated gelation behavior, ionogel precursors consisting of poly(ethylene glycol) diacrylate and 1-butyl-3-methylimidazolium tetrafluoroborate experience in situ confined polymerization and gelation within CNTs-stacked skeleton, thus making free ILs dually locked via dual confinement of CNTs skeleton and gel network. These DCIMs have a greatly decreased thickness to 1–3 µm by ≈100 folds over counterparts, yet exhibiting an enhanced pressure resistance and long-term stability. Moreover, DCIMs give an ultrahigh CO 2 permeance of 113 GPU, a rewarding CO 2 /N 2 and CO 2 /CH 4 selectivity of 68 and 88, respectively, transcending most ILs-based membranes. These findings represent a paradigm shift in developing advanced ionogel membranes beyond gas separation.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Yang Chen,Diwen Zhou,Yongli Chang,Hongqiao Lin,Yunzhao Xu,Yong Zhang,Ding Yuan,Lizhi Wu,Yu Tang,Chengyi Dai,Xingang Li,Qinhong Wei,Li Tan
CO 2 hydrogenation to CH 3 OH is of great significance for achieving carbon neutrality. Here, we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts (CZC-G) with optimized interfacial synergy, achieving superior performance in CO 2 hydrogenation to methanol. The CZC-G catalyst demonstrated exceptional methanol selectivity (96.8%) and a space-time yield of 73.6 g MeOH ·kg cat –1 ·h –1 under optimized conditions. Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation. Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-O v -Ce ternary interfaces and inhibits the reduction of ZnO, enabling synergistic interactions for efficient CO 2 activation and selective stabilization of formate intermediates (HCOO*), which are critical for methanol synthesis. In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism, while suppressing the reverse water-gas shift reaction. This work underscores the critical role of synthetic methodologies in engineering interfacial structures, offering a strategy for designing high-performance catalysts for sustainable CO 2 resource utilization.
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JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Po-Chun Wu,Ho Jun Lee,Yi-Fan Lin,Kuo-Lun Tung,Jong Suk Lee,Dun-Yen Kang
Carbon capture is widely recognized as a pivotal technology for alleviating the accelerating impacts of global warming. Mixed matrix membranes (MMMs) that embed metal organic frameworks (MOFs) offer a compelling route to high-performance separations, and MOF-808 stands out among them because of its outstanding chemical stability and environmentally friendly synthesis. In this study, the defect density of MOF-808 was tuned by varying the formic acid modulator: Higher modulator loading produced MOF-808 with higher linker defect density. After synthesis, MOF-808 was washed with either water or ethanol and then incorporated into PEBAX matrix through a drying-free process that ensured uniform dispersion. Washing with ethanol altered the pore coordination environment of MOF-808, partially replacing formate with ethoxide. Introducing an appropriate amount of formic acid created additional open metal sites and increased both CO 2 permeability and CO 2 /N 2 selectivity; however, excessive formic acid produced too many defects, causing severe pore blockage and consequently lowering the CO 2 permeability. The drying-free method, by preventing MOF aggregation and ensuring homogeneous dispersion, led to a 38 % increase in CO 2 /N 2 selectivity compared with the conventional drying method. The ethoxide substitution induced by ethanol washing occupied part of the pore volume, leading to a reduction in CO 2 permeability. The optimized MOF-808/PEBAX MMM achieved a CO 2 permeability of 150 Barrer and a CO 2 /N 2 selectivity of 76.4, both markedly higher than those of the pristine polymer. These results highlight a sustainable, scalable strategy for producing high-efficiency membranes for post-combustion CO 2 capture.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
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IF 15.7
Li Hao-Nan,Sun Ze-Yu,Yu Zhen-Jie,Man Kexin,Zhang Chao,Xu Zhi-Kang
Mixed matrix membranes (MMMs) capable of breaking the permeability-selectivity trade-off suffer from the inefficient and disconnected bulky transport channels as well as inferior interfacial compatibility between nanomaterials and polymers. Herein, we propose an original photothermal-triggered in-situ gelation approach to elaborate an original class of MMMs, termed nanofiber-interwoven gel membranes (NIGMs) that feature tunable 3D-interconnected ultrafast transport channels and highly-selective CO 2 -philic gel for boosting CO 2 separation performance. The key design of NIGMs lies in leveraging dual functions of CNT-interwoven skeleton: (1) serving as a photothermal confined reactor that rapidly triggers in-situ gelation of highly-selective CO 2 -philic gel without phase separation-induced interfacial defects to construct defect-free and thickness-controllable NIGMs; (2) functioning as a 3D-interconnected continuous skeleton for providing ultrafast CO 2 transport channels. By orchestrating the distribution and configuration of interwoven nanofibers, the NIGMs possess a boosted CO 2 permeance of 211.0 GPU increased by 1558% over polymeric gel counterparts and an ultrahigh CO 2 /N 2 and CO 2 /CH 4 selectivity of up to 151 and 47 respectively. Our work offers a paradigm shift in developing advanced MMMs beyond gas separation.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Gong Shanhe,Zhai Yanjie,Jin Chengkai,Xu Han,Xia Qing,Li Weisong,Ying Yiran,Wu Jie,She Xiaojie,Wang Zhaolong,Lv Xiaomeng,Wu Chundu,Chan Kangcheung,Zhao Xunhua,Zhang Xiao,Lau Shu Ping
Electrochemical carbon dioxide reduction reaction (CO 2 RR) under strongly acidic conditions enables high CO 2 utilization. However, especially in proton exchange membrane (PEM) electrode assembly reactors, achieving selective CO 2 RR in such environments remains challenging due to uncontrolled interfacial water diffusion at high current densities. Here, we develop a nickel-based heterogeneous molecular electrocatalyst (NiPc-NH 2 /CNT-SHP) featuring amino (-NH 2 ) functional groups and grafted long-chain hydrophobic molecules. Under acidic conditions, -NH 2 is in situ protonated to form amino cations (-NH 3 ⁺). The positively charged -NH 3 ⁺ groups and hydrophobic molecules effectively disrupt the protonated water (H 3 O + )-rich network, inhibiting the invasion of H 3 O + and thereby suppressing the hydrogen evolution reaction, while enhancing selectivity for acidic CO 2 RR. The catalyst achieves nearly 100% Faradaic efficiency for CO at current densities from 50 to 400 mA cm −2 , with approximately 76% CO 2 utilization efficiency in a flow cell, and sustains over 80% selectivity for more than 200 h in a self-designed PEM–porous solid electrolyte reactor. These findings highlight interfacial water management as a key design principle for efficient acidic CO 2 electroreduction.
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THERMOCHIMICA ACTA
·
2025
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IF 3.5
Wenke Zhang,Jianzhong Liu,Haiou Wang,Xueqin Liao,Jianren Fan
Aluminum (Al) combustion in CO 2 was investigated to assess carbon sequestration potential. Theoretical and experimental results identified C(s), Al 4 C 3 (s), and CO(g) as primary products, with C(s) formation being most thermodynamically favorable. Al oxidation in CO 2 proceeded through three stages, with the second stage (activation energy: 260–268 kJ·mol⁻¹) exhibiting the highest reactivity. Kinetic analysis indicated an Anti-Jander/D1 mechanism for this dominant stage. Reducing particle size from 25 μm to 0.1 μm at 0.1 MPa shortened ignition delay by 664 ms and increased combustion temperature by 847 K. Characterization confirmed carbon incorporation in products (Al 2 O 3 /Al 4 C 3 ) and demonstrated enhanced combustion efficiency and carbon fixation with smaller particles or higher pressures. These findings provide critical insights for Martian in-situ resource utilization and carbon capture technologies.
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