Catalysts
·
2025
·Vol. 15
·期 7
·623
·
IF 4
Caidong Du,Wenwei Wu,Jiangtao Shang,Keyi Xiang
Methane (CH4) has attracted much attention regarding its use in electrochemical carbon dioxide reduction reaction (CO2RR) due to its high mass-energy density; however, the uneven adsorption of intermediates on copper sites by conventional Cu-based catalysts limits the selective production of CH4. The introduction of a second metal can effectively regulate the adsorption energy of intermediates on the Cu site. In this paper, a method of alloying Cu with oxyphilic metals (M) using rapid electrodeposition is presented; the synergistic effect of the bimetal effectively directed the reaction pathway toward CH4. The best Faraday efficiency for methane occurred in the optimized Cu30La20electrode, reaching 66.9% at −1.7 V vs. RHE potential. In situ infrared testing revealed that the *CHO intermediate—a critical species for the electrocatalytic conversion of CO2to CH4—was detected on the Cu30La20catalytic electrode. However, no *CHO intermediate was observed on the Cu20La30electrode. Instead, the characteristic peak of the *OCCHO intermediate associated with C-C coupling emerged on the Cu20La30catalyst. This indicates that the adsorbed oxygen-containing groups on lanthanum sites reacted with carbon-containing groups on copper sites to form C2products, serving as the primary reason for the shift in reduction products from methane to ethylene.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Jiale Ni,Zicheng Yang,Binxuan Hong,Yi Feng,Jianfeng Yao
This research endeavors to optimize the morphology and edge defects of g-C 3 N 4 through straightforward pyrolysis of rationally chosen precursors, with the objective of increasing the CO 2 conversion efficiency. Our findings reveal that employing melamine and urea as precursors yields tubular g-C 3 N 4 (CN tube), featuring an increased surface area and a greater density of edge defects than melamine-derived bulk g-C 3 N 4 and urea-derived layered g-C 3 N 4 . As a result, the obtained CN tube can deliver an impressive yield of 98 % for CO 2 cycloaddition with epichlorohydrin at 12 h under mild conditions of 80 °C and 0.1 MPa CO 2 pressure, significantly outperforming those derived from melamine (53 %) or urea (66 %) alone. This investigation demonstrated the pivotal role of a tubular architecture and enriched edge defects in facilitating the thermally driven CO 2 fixation process to produce cyclic carbonates.
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ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Wenlong Wang,Wentao Hao,Lang He,Jia Qiao,Ning Li,Chaoqiu Chen,Yong Qin
S-scheme heterojunctions have garnered significant interest in photocatalytic CO 2 conversion to valuable products (e.g., CH 4 ) due to their enhanced charge separation and robust redox capabilities. Carbon dots (CDs), with their tunable band structures and light absorption ranges, show particular promise in constructing efficient S-scheme photocatalytic systems. Nevertheless, the critical roles of CDs' band alignment and surface adsorption properties in determining heterojunction configuration, charge carrier kinetics, and ultimately CO 2 activation/product selectivity distribution remain insufficiently explored. Herein, we construct four CDs/TiO 2 heterojunctions using CDs synthesized from varied carbon sources, in which S-scheme heterojunctions were successfully constructed based on cost-effective coal pitch (C-GQDs, 1.75 nm), glucose (G-CQDs, 1.84 nm), and acetone (CQDs-X, 1.82 nm) carbon sources, whereas Type-I heterojunctions were formed by carbon black based CDs (GQDs-A, 1.92 nm). Systematic investigations reveal that both the band structure and adsorption characteristics of CDs play important roles in the charge transfer path and separation efficiency, CO 2 adsorption and activation capacities, and product selectivity in photocatalytic CO 2 reduction. Remarkably, the introduction of CDs significantly broadens the photo-response range compared to fresh TiO 2 , and in particular, the C-GQDs/TiO 2 exhibits exceptional performance with a CH 4 production rate of 32.7 μmol·g −1 ·h −1 , surpassing TiO 2 by 6.3-fold and outperforming GQDs-A/TiO 2 , CQDs-X/TiO 2 , and G-CQDs/TiO 2 by factors of 3.8, 2.7, and 2.3, respectively. This heterojunction simultaneously achieves 72.6 % CH 4 selectivity and 98.1 % hydrocarbons selectivity (encompassing CH 4 , C 2 H 6 , C 2 H 4 , and C 3 H 8 ). In contrast, composites incorporating GQDs-A, CQDs-X, or G-CQDs exhibit substantially diminished CH 4 selectivity (<40.0 %). The high CH 4 production rate and selectivity of C-GQDs/TiO 2 can be attributed to its unique S-scheme heterojunction structure, higher reduction potential, and well-matched CO 2 and H 2 O adsorption and activation capabilities. This study provides unique insights into the efficient photoreduction of CO 2 to CH 4 driven by the S-scheme heterojunction electron transfer pathway in CDs/TiO 2 photocatalysts.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Liuliu Zhong,Qisheng Hu,Changjian Li,Jing Ding,Chundong Zhang,Hui Wan,Lei Wang,Guofeng Guan
The hydrogenation of CO2 to produce α-olefins and other high-value chemicals plays a crucial role in energy transformation and sustainable low-carbon development. However, the CO2 hydrogenation pathway for α-olefin synthesis still encounters various challenges, such as limited CO2 conversion and low α-olefin selectivity. To tackle these issues, this study initially assessed the catalytic properties of iron-based catalysts with varying morphologies and particle sizes. The findings indicated that the spherical Fe3O4 catalysts with large specific surface area demonstrated high CO2 conversion (20.8%) and α-olefin selectivity (14.4%) To improve CO2 adsorption and facilitate carbon chain growth, K and Sr were introduced to modify the spherical Fe3O4 catalysts. The synergistic electronic and structural effects of K and Sr contributed to enhanced α-olefin formation. Experimental data revealed that, under reaction conditions of 340 °C, 2.5 MPa, and a space velocity of 5000 h–1, the optimized 5K10Sr/Fe3O4 microsphere catalyst achieved a CO2 conversion of 45.4%, C2+ selectivity of 68%, chain growth factor of 0.67, and LAO (linear α-olefins in C4+ products) selectivity of 53.6%.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xiongwei Tian,Zheng Chen,Francesco Iacoviello,Mengyin Xie,Wenqing Chu,Yuqun Zhuo
The electroreduction of carbon dioxide (CO2R) presents a promising avenue for mitigating CO2 emissions while producing valuable chemicals. In this work, we report a novel pressure equilibrium strategy tailored for pressurized CO2R in a zero-gap electrolyzer, aiming at accommodating the high-pressure CO2 sources from its capture, utilization, and storage scheme. We investigated the impact of pressure on the CO2R performance under both gaseous and supercritical conditions, while also examining the synergistic interplay of temperature with high pressure. Significant enhancement of energy efficiency (46.5%) with high CO Faradaic efficiency (94.4%) and low cell voltage (−2.72 V) was achieved at 200 mA/cm2 under 75 bar and 80 °C. In addition, we noticed that the agglomeration and migration of salt precipitation within the gas diffusion electrode were effectively suppressed under pressurized conditions, which indicated the potential benefit for prolonged cell stability.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaohui Sun,Linglong Wang,Yongxiao Tuo,Bangyan Zhang,Tao Gan,Jiansong Miao,Chunming Xu
Renewable-driven electrochemical reduction of CO 2 (CO 2 RR) to syngas is an attractive approach to achieve carbon neutrality. However, high current density at specific H 2 /CO molar ratios is challenging. Herein, a sulfur, nitrogen co-doped carbon supported Ni an Co dual-atom-system is designed as electrocatalyst to produce syngas from CO 2 RR. By regulating the molar ratio of Co and Ni in the dual atom system, H 2 /CO molar ratios of 1 and 2 that are typically suitable for a downstream Fischer-Tropsch synthesis process can be controlled in a wide current density range from 50 to 250 mA/cm 2 . This is attributed to the fact that single Ni sites are highly active for CO 2 RR to CO, while single Co sites are highly active for H 2 production. Moreover, experiments combined with theory confirm the presence of a sulfur-bridged Co and Ni moiety in the dual-atom system, and electrons are transferred from the Co and neighboring Ni sites to the bridged S atom. These electron deficient Co and Ni sites efficaciously balanced the adsorption strength of COOH* and H*, further facilitating syngas production without scarifying total current densities. This study provides a useful case for the fabrication of dual-atom catalysts with industrial relevant syngas production via CO 2 RR.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Liang Ye,Siyang Jin,Ke Yang,Jianchao Zhou,Hang Wu,Yue Jiang,Wei Xu
A high-entropy lanthanide-based metal-organic framework (HE-LnMOF), integrating five distinct lanthanide ions (Eu 3 ⁺, Tb 3 ⁺, Gd 3 ⁺, Dy 3 ⁺, Ho 3 ⁺) and 2-aminoterephthalic acid (H 2 N-BDC) ligands, was solvothermally synthesized for efficient catalytic conversion of CO 2 into cyclic carbonates. Structural analyses confirmed the homogeneous distribution of lanthanide ions within the framework, inducing lattice distortion while preserving crystallinity. The material features uncoordinated amino groups acting as base sites and unsaturated metal centers serving as Lewis acid sites, synergistically enhancing CO 2 adsorption and activation. HE-LnMOF demonstrated superior catalytic performance for converting CO 2 into cyclic carbonates compared to monometallic Ln-MOF analogs. In situ DRIFTS studies revealed intensified carbonate intermediate signals, corroborating the role of cooperative acid-base sites in accelerating the reaction. This work demonstrates the potential of high-entropy design in MOFs to amplify catalytic efficiency and stability, offering a sustainable pathway for CO 2 utilization.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xixuan Hu,Liang Huang,Chengbo Zhao,Qiang Wang
Although minerals-derived Li 4 SiO 4 demonstrates enhanced CO 2 capture performance and cost-effectiveness, the specific impurity-derived dopants governing cyclic stability and sorption kinetics still remain poorly understood. In this contribution, we reveal that Al doping (Si/Al = 3.76–5.68) improves cyclic stability by serving as both structural separator and support, while Na doping (Si/Na ≤20.6) enhances sorption capacity and kinetics. DFT simulations confirm Al reduces surface energy while Na increases exposure facet adsorption energy. Perlite is selected as the optimal silicon source from six minerals, and the derived perlite-Li 4 SiO 4 demonstrates superior CO 2 sorption capacities of 33.9 wt% at 650 °C and 8.3 wt% at 400 °C under 100 vol% CO 2 , maintaining 92% initial capacity even under low CO 2 concentrations (20%). Remarkable regeneration stability is observed through 100 cycles with only 1.7 wt% capacity loss. Lower activation energy (chemisorption phase) and 1.73 GJ/t CO 2 regeneration heat confirm its industrial viability. The impurity-doping synergism elucidates a self-reinforcing rationale for engineering stable high-temperature CO 2 capture materials with operational durability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Ruxing Gao,Xixi Chen,Chao Deng,Lujing Xu,Leiyu Zhang,Chundong Zhang,Ki-Won Jun,Tiansheng Zhao,Yingju Yang
Catalytic hydrogenation of CO 2 into light olefins has gained increasing attention, nevertheless the design of an efficient catalyst with high selectivity towards light olefins is still challenging. Herein, aiming at improving the selectivity of targeted light olefins, we successfully synthesized a series of Na/MFe 2 O 4 (M = Co, Zn and Cu) spinel catalysts via hydrothermal synthesis, and tried to establish their activity-structure relationship. Among the Na/MFe 2 O 4 spinel catalysts, the Na/CoFe 2 O 4 catalyst shows superior catalytic performance, thanks to the well-crystallized CoFe 2 O 4 nanoparticle which has the good dispersibility, reducibility and carburizing ability. Moreover, compared with the traditional Na/Fe–Co catalyst obtained via co-precipitation, the formation of CoFe 2 O 4 with uniform crystal phase and smaller crystal size for Na/CoFe 2 O 4 spinel catalyst is more conducive to the formation of active and stable χ-(Co x Fe 1 − x ) 5 C 2 alloy carbide, thereby resulting in excellent catalytic activity and stability. On this basis, to further improve the C 2-4 = selectivity, we coupled the Na/CoFe 2 O 4 component with acidic zeolites (e.g., SAPO-34, MOR and Hβ), and the Na/CoFe 2 O 4 @SAPO-34 catalyst is found to possess a superior C 2-4 = selectivity of 42 % with a CO 2 conversion of 39 %. This work can provide a useful understanding of designing efficient spinel-structured bimetal catalysts for selective conversion of CO 2 into value-added light olefins.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yan Huang,Yujia Liu,Yi Liu,Xinqiu Tan,Yikai Wang,Qian Xiao,Xiaoyu Tong,Jinghui Pan,Zebin Yu,Zuofang Yao,Yanping Hou
Lead-free halide double perovskites (LFHDPs) show great potential for solar-to-fuel conversion due to their unique photoelectrochemical properties, but they suffer from easy carriers recombination and insufficient active sites. In this work, a series of Co-doped Cs 4 MnBi 2 Cl 12 (denoting as Cs 4 MnCo x Bi 1-x Cl 12 ) microcrystals were synthesized for CO 2 photocatalytic reduction. Results of various characterizations, Kelvin probe microscopy mode (KPFM) and density functional theory simulation (DFT) calculations showed that Co doping into the Cs 4 MnBi 2 Cl 12 could induce spin polarization, resulting in fast carriers separation and extending carriers lifetime. The Cs 4 MnCo 0.9 Bi 0.1 Cl 12 (CMC 0.9 B 0.1 C) microcrystals exhibited the CO yield of 69.16 μmol·g −1 ·h −1 , which was 177 times of that of CMBC (0.39 μmol·g −1 ·h −1 ). Notably, CO 2 reduction performance from the CMC 0.9 B 0.1 C was significantly enhanced by applying an external magnetic field (300 mT) to the system, with CO yield reaching 99.96 μmol·g −1 ·h −1 . The main intermediates during CO 2 reduction were carboxylate (COOH*) and chelating-bridged carbonate (C-CO 3 2− ), and CO 2 reduction pathways and mechanism were proposed accordingly. These findings highlight the great potential of Co-doped Cs 4 MnCo x Bi 1-x Cl 12 as a promising photocatalyst for light-driven CO 2 reduction, opening up new avenues for the development of LFHDPs-based photocatalytic system.
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JOURNAL OF POLYMER SCIENCE
·
2025
·
IF 3.6
Dake Zhang,Wenzhen Wang,Dengmeng Song,Xingang Jia,Dingyuan Deng,Jingyu Wang,Xinyi Wang,Li Xia
While organogel adsorbent resins demonstrate excellent performance in organic pollutant separation, their limited reusability and high carbon footprint significantly restrict further development and application. Addressing the urgent environmental challenge of CO 2 emissions, we leveraged the inherent biodegradability and eco-compatibility of CO 2 -derived poly(propylene carbonate) (PPC) to synthesize a series of highly crosslinked PPCG materials by incorporating glycidyl methacrylate (GMA)—a monomer featuring carbon–carbon double bonds, ester groups, and epoxy functionalities—during terpolymerization. The introduced ester groups facilitate chemisorption and enhanced diffusion of lipophilic organics. Studies confirmed PPCG's exceptional adsorption capacity for chloroform, benzene, toluene, and tetrahydrofuran (THF), achieving a remarkable 977% swelling ratio for chloroform. After 8 adsorption–desorption cycles, all PPCG variants (PPCG1–PPCG5) retained > 95% adsorption efficiency. Thermal and mechanical analyses further validated that increased crosslinking density improved material stability. This green, reusable organogel adsorbent addresses the critical gap in applying CO 2 -based polycarbonates to separation technologies, establishing a novel functionalization strategy for next-generation adsorbent design. Graphical Schematic illustration of the synthesis process and working mechanism of organic gel adsorption resin.
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WATER SCIENCE AND TECHNOLOGY
·
2025
·Vol. 92
·期 1
·127-138
·
IF 2.6
Wang Wei,Li Haoxuan,Xie Yue,Zhao Yingying,Xiong Rihua
Climate change demands innovative carbon capture and utilization (CCU) strategies, yet converting captured CO 2 into high-value products while managing industrial waste remains elusive. Here, we demonstrate a single-step, energy-efficient bipolar membrane electrodialysis (BMED) system integrated with CCU, enabling the simultaneous conversion of NaCl brine and CO 2 into high-purity sodium bicarbonate (NaHCO 3 ) with unprecedented efficiency, but without requiring external alkali sources or energy-intensive thermal regeneration steps. By optimizing key parameters – such as current density and CO 2 aeration rate, and gas–liquid flow ratios – we achieved a bicarbonate concentration of 1.186 mol/L in the alkaline chamber, coupled with 57.65% carbon sequestration efficiency and an energy consumption as low as 3.1 kW·h/m³ CO 2 (or 716.9 kW·h/t NaHCO 3 ). This approach not only recovers valuable sodium resources from brine but also enhances CO 2 absorption through electrochemical mechanisms, potentially reducing global carbon emissions by up to 20% in brine-intensive industries. Our work paves the way for scalable, sustainable CCUS technologies, transforming waste streams into economic assets and advancing the fight against climate change. Integration of BMED with CO 2 sequestration for NaHCO 3 production from NaCl brine. Energy-efficient and sustainable CO 2 utilization for marketable products. Optimization of key operational parameters for improved efficiency.
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高影响因子
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