APPLIED CATALYSIS A-GENERAL
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2026
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IF 4.8
Siyu Yi,Guobin Zhou,Yi Wang,Mengxia Ji,Jinman Yang,Yi Zhang,Pengcheng Yan,Zhao Mo,Zhaolong Wang,Junjie Yuan,Hui Xu,Xiaojie She
Electrocatalytic CO 2 methanation is promising for carbon neutrality but hindered by complex multi-electron transfer process, thereby obtaining low product selectivity. Herein, we report a copper single atom catalyst anchored on nitrogen doped carbon nanotubes (Cu-N-CNTs) for efficient electrocatalytic CO 2 methanation. By synergistically regulating the precursor, Cu-N 4 active sites are precisely constructed at the atomic scale, effectively suppressing copper aggregation. In situ characterization indicates that the catalyst forms a moderate local alkaline microenvironment during the reaction, suppressing C-C coupling side reactions and promoting methane pathways. In the flow cell, Cu-N-CNTs achieve a FE CH4 of 59.2% and a partial current density of 168.7 mA cm −2 at −1.577 V vs. RHE, and operated stably for 10 h. Moreover, Cu-N-CNTs exhibit remarkable methane selectivity in membrane-electrode assembly (MEA) systems employing both alkaline and pure-water electrolytes. A scaled-up MEA prototype further verifies the outstanding operational stability of Cu-N-CNTs under practical conditions. These results collectively underscore the substantial potential of Cu-N-CNTs for industrially relevant electrocatalytic CO 2 methanation.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2018
·
IF 1.712
Jing Zhu,Lisong Fan,Lina Song,Fengqiu Chen,Dangguo Cheng
Developing effective iron-incorporated zeolites and determining their active centers for the direct oxidation of CH 4 to oxygenates have remained challenging topics so far. In this paper, we successfully prepare the highly-dispersed iron supported Y zeolites by a facile solid-state ion-exchange method with ferrocene, which was conducted under water-free conditions followed by a series of calcination . Moreover, extra-framework dinuclear Fe 2 + complexes are identified as so-called active α-iron sites on zeolites. ICP-OES, N 2 adsorption–desorption test, X-ray diffraction, solid-state 27 Al NMR, N 2 O titration, TEM, EPR and 57 Fe Mössbauer spectra were carried out to characterize properties of sample structure, acid sites, as well as the supported iron species. Characterization results indicate that high-temperature treatments have no effect on the typical structure feature of zeolites. Compared with catalysts synthesized by conventional impregnation, the samples prepared by the facile approach possess abundant dinuclear Fe 2 + complexes but no Fe 2 O 3 bulks and show weak acidity. These lead to a higher oxygenate selectivity in CH 4 oxidation to oxygenates. Remarkably, the oxygenate (HCHO and CH 3 OH) selectivity of 6.5% at 375°C can be eventually obtained.
研究领域:
催化化学
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材料科学
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Nano Research
·
2017
·Vol. 10
·期 10
·3396-3406
·
IF 7.354
Zhu Yuzhen,Gao Chao,Bai Song,Chen Shuangming,Long Ran,Song Li,Li Zhengquan,Xiong Yujie
Photocatalytic reduction of CO 2 into high value-added CH 4 is a promising solution for energy and environmental crises. Integrating semiconductors with cocatalysts can improve the activities for photocatalytic CO 2 reduction; however, most metal cocatalysts mainly produce CO and H 2 . Herein, we report a cocatalyst hydridation approach for significantly enhancing the photocatalytic reduction of CO 2 into CH 4 . Hydriding Pd cocatalysts into PdH 0.43 played a dual role in performance enhancement. As revealed by our isotopic labeling experiments, the PdH 0.43 hydride cocatalysts reduced H 2 evolution, which suppressed the H 2 production and facilitated the conversion of the CO intermediate into the final product: CH 4 . Meanwhile, hydridation promoted the electron trapping on the cocatalysts, improving the charge separation. This approach increased the photocatalytic selectivity in CH 4 production from 3.2% to 63.6% on Pd{100} and from 15.6% to 73.4% on Pd{111}. The results provide insights into photocatalytic mechanism studies and introduce new opportunities for designing materials towards photocatalytic CO 2 conversion.
研究领域:
材料科学
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环境科学
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Materials Today Nano
·
2023
·
IF 10.3
L.K. Pan,J.C. Qi,H. Mei,L. Yao,H.X. Liu,S.X. Zhou,G.Q. Zhu,J.J. Wang,L.F. Cheng,L.T. Zhang
Developing efficient and highly selective photocatalytic CO 2 reduction catalysts remains one of the most significant challenges in achieving carbon neutrality . Herein, the efficient conversion of CO 2 to CH 4 with selectivity close to 100% was achieved by loading uniformly dispersed Pt nanoparticles on the surface of Sr 2 Nb 2 O 7 nanosheets ; the optimal CH 4 yield was as high as 15.65 μmol/g/h. Various characterizations demonstrate that Pt nanoparticles have a significant photothermal effect that can increase the catalyst surface temperature, and improve the performance and electron transport rate of the catalyst. Additionally, Pt nanoparticles and Sr 2 Nb 2 O 7 nanosheets form heterojunctions , which facilitate the separation of photogenerated carriers and aggregation of photogenerated electrons on the Pt nanoparticles. Pt nanoparticles become new reactive sites that have a strong adsorption impact on the key intermediate ∗CO and reduce the reaction energy barrier of ∗CHO generation. The results revealed that the synergy between electron accumulation, strong adsorption of ∗CO, and reduction of the reaction potential of ∗CHO are the reasons for the efficient and selective conversion of CO 2 to CH 4 . This work provides novel insights into the role of metal-based cocatalysts in selective CO 2 photoconversion and new ideas for designing efficient CO 2 conversion systems.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Mengmeng Ni,Lihong Wang,Yao Chai,Bing Wang,Dongmiao Li,Jinni Shen,Zizhong Zhang,Xuxu Wang
The photocatalytic conversion of CO 2 and H 2 O into a series of value-added products is regarded as an important way to mimic natural photosynthesis for solar harvesting. Herein, we prepared CsBi 2 Ta 5 O 16 with a cubic pyrochlore structure via high-temperature molten salt method as a photocatalyst for the first time. The NiO-loaded CsBi 2 Ta 5 O 16 composites could efficiently photocatalyze the conversion of CO 2 into CH 4 and CO, and oxidize H 2 O to O 2 . With 10 wt% NiO loading, the highest yield of CH 4 (7.24 μmol g −1 h −1 ) and O 2 (3.59 μmol g −1 h −1 ) could be achieved. The adsorption and activation of CO 2 molecule on NiO can be attributed to the enhanced CO 2 photocatalytic conversion by the NiO-loaded CsBi 2 Ta 5 O 16 composites. This work provides a design idea of photocatalyst for the full reaction of CO 2 with H 2 O.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zongze Lv,Changlei Qin,Shuzhen Chen,Dawid P. Hanak,Chunfei Wu
CO 2 capture and utilization has been considered as an up-and-coming short- to mid-term approach to mitigate the excessive CO 2 emission. Comparing to the conventional separate capture, transportation and conversion arrangement, the integrated CO 2 capture and utilization (ICCU) could largely simplify the complex process and reduce the energy consumption. However, the poor stability of high-temperature CO 2 sorption/desorption severely limit the potential of ICCU. Therefore, it is indispensable to develop a new sorbent/catalyst system ensuring the high-efficiency and long-term operation of the ICCU. In this paper, we propose and demonstrate the feasibility and performance of using K 2 CO 3 -doped Li 4 SiO 4 as an efficient CO 2 sorbent for ICCU operating at a relatively low temperature by dry reforming of methane. Results show that the ratio of H 2 /CO produced is stabilized at 1 ± 0.05 in the pre-breakthrough stage, and the duration extends to be 1.6 times of the original value in the cyclic operations, displaying an excellent performance in reaction matching and process stability.
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Korean Journal of Materials Research
·
2025
·Vol. 35
·期 8
·352-365
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IF 0.3
Haixia Wang,Yilei Sun,Yao Liu,Kunjie Li,Zeda Meng,Won-Chun Oh
The catalyst materials 0N-Cu-MOF, 1N-Cu-MOF, and 2N-Cu-MOF were successfully synthesized usinga solvothermal method, and using different concentrations of nitrogen-modified Cu organic frameworks (xN-Cu-MOF). Characterizations using X-ray diffraction (XRD), scanning electron microscopy (SEM), fourier transform infrared (FT-IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) surface area analysis showed that 1N-Cu-MOF had the largest SSA and pore size among the three materials synthesized. 1N-Cu-MOF exhibited the largest pore size and specific surface area among the three materials, which had a decisive effect on CO2 reduction. In addition, stability and CO2 reduction reaction (CO2RR) activity were evaluated by linear sweep voltmeter, cyclic voltmeter, electrochemical impedance spectroscopy, and time flow tests. Faradaic efficiency (FE) was determined by product analysis. Among the three catalyst materials, 1N-Cu-MOF showed the best catalytic performance at 50 mA·cm-2 (maximum current density). The charge transfer resistance was 8.23 Ω, the average current density was 19.9 mA·cm-2, and the FE of methane (CH4) production showed a high efficiency of 70.45 % when tested for 12 h at an overpotential of -0.35 V (to-RHE).
研究领域:
材料化学
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电化学
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环境催化
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能源材料
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纳米催化
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PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2012
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IF 1.693
Jiangfeng Yang,Qiang Zhao,Hong Xu,Libo Li,Jinxiang Dong,Jinping Li
We prepared several different surfaces and pore volumes on small pore zeolites by hydrothermal synthesis and ion exchange (Li+, Na+, and Ca2+) based on three basic gas diameter grade structures of zeolites: KFI (0.39 × 0.39 nm), CHA (0.38 × 0.38 nm), and LEV (0.36 × 0.48 nm), which were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and elemental analysis. The surface area and microporous volumes were calculated using the Dubinin–Radushkevitch (D-R) equation based on CO2 adsorption at 273 K. The CHA was synthesized with a lower Si/Al ratio, and the surfaces and microporous volumes were changed greatly by ion exchange. KFI had a higher Si/Al ratio, and the scope of the surface could be kept smaller. Focusing on the CO2, CH4, and N2 adsorption isotherms at high pressure (1 MPa), we found that the samples were exchanged by Li+ and Na+ with bigger surfaces and greater adsorption volumes. The orifice diameter was very important in the sieving of CO2 and N2 or CO2 and CH4, while Na-LEV had an excellent sieving effect because N2 and CH4 could not diffuse into its structure like CO2. From the viewpoint of the separate adsorption equilibria: Na-zeolites had the highest data adsorption equilibrium selectivity for CO2 and N2 or CO2 and CH4, followed by Li-zeolites, which only had a strong adsorption potential of CO2; K-zeolites with high SCO2/N2 and SCH4/N2, based on the strong adsorption of CO2 and CH4. We conclude that the adsorption potential order was K-zeolites > Na-zeolites > Li-zeolites, so the bigger ions had a stronger affinity.
研究领域:
材料科学
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吸附与分离技术
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化学工程
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多孔材料
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环境科学
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ACS Sustainable Chemistry & Engineering
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2026
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IF 7.6
Jiahui Zhou,Ziyi Zhang,Chenghao Jin,ShanShan Tong,Yunteng Qu
Electrochemical CO2 reduction reaction (CO2RR) to diverse high-value chemicals represents a promising carbon mitigation strategy, yet precisely controlling product selectivity remains a considerable challenge. Herein, we report a size-dependent Cu/CN catalyst for modulating the selectivity of CO2RR. Specifically, small Cu NPs on CN (∼5 nm, S–Cu/CN) achieved a 76.2% C2+ product selectivity at 0.6 A cm–2, while the large one (∼50 nm, L-Cu/CN) reached a 67.5% CH4 selectivity at 0.6 A cm–2. Physical characterizations revealed that S–Cu/CN displays partial Cu+ sites, whereas L-Cu/CN higher Cu+ content. Mechanism analysis revealed a balanced Cu0/Cu+ ratio in S–Cu/CN promotes C–C coupling at Cu+ sites to form C2+ products. Conversely, higher Cu+ content in L-Cu/CN decreased the *CO coverage and improved H2O dissociation, steering continuous hydrogenation toward CH4 generation. This work offers a novel strategy to design high-efficiency CO2RR electrocatalysts toward desired products.
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ACS Applied Engineering Materials
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2026
·
IF 3.5
Luo Dan,Wang Rui,Chang Tong,Jia Lijuan,Li Dong,Lu Kuan,Wei Yuxue
The Fischer−Tropsch synthesis (FTS), the key industrial process for the transformation of syngas into valuable chemicals and clean fuels, benefits from advanced catalyst design. Iron carbide nanoparticles (Fe 3 C) and their graphene oxide-derived counterpart (Fe 3 C/Graphene) were successfully synthesized. Fe 3 C/Graphene exhibits a large specific surface area, high pore volume, and abundant surface defective sites provided by the reduced graphene oxide support. Together with the stabilized Fe 3 C active phase, these features promote CO activation and C−C coupling, leading to enhanced CO conversion, higher C 5+ selectivity, and suppressed CH 4 formation comparedwith Fe 3 C. Density functional theory calculations reveal that the improved CO activation on Fe 3 C/Graphene originates from reduced electron transfer and weakened Fe−C and C−O bonds. For Fe 3 C, the rate-determining step is CO* + H* → CHO*, whereas for Fe 3 C/Graphene, the rate-determining step is CHO* → CH* + O*. It also reveals that Fe 3 C/Graphene accelerates this step, corroborating the enhanced CO activation observed experimentally. Furthermore, the simulations confirm that defective graphene significantly raises the effective barrier for methanation, perfectly rationalizing the suppressed CH 4 formation. These findings demonstrate that the introduction of graphene oxide is a effective strategy for tailoring the catalytic performance of Fe-based FTS catalysts.
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MOLECULES
·
2026
·Vol. 31
·期 13
·2304
·
IF 5.1
Haopeng Cui,Zhiying Li,Siyu Huang,Tianyi Zhang,Xiaodong Zhang,Zhongxiao Zhang,Jianqiu Lei,Ning Liu
Photocatalytic CO2reduction into CH4is a promising route for solar fuel production, but its efficiency is still limited by poor charge separation, insufficient CO2activation, and sluggish multi-electron transfer kinetics. Herein, Cu-modified TiO2(Cu/TiO2) was prepared by calcining a Cu-modified defective MIL-125(Ti) precursor, denoted as Cu-MIL-125, through a temperature-controlled calcination strategy. The effects of calcination temperature on the structural evolution, surface chemical states, interfacial charge transport, and CO2photoreduction performance were examined. These results indicated that the Cu/TiO2was successfully prepared, while the crystallinity, porous structure, and interfacial electronic properties of Cu/TiO2were strongly dependent on the calcination temperature. Among the obtained samples, the Cu/TiO2sample obtained by calcining Cu-MIL-125 at 450 °C (450 Cu/TiO2) exhibited the highest CH4formation rate, reaching 15.90 μmol g−1h−1, corresponding to an approximately 9.8-fold enhancement over TiO2calcined from defective MIL-125(Ti) at 450 °C, together with a high CH4selectivity of 93.05%. Control experiments and13CO2isotope-labeling tests confirmed that the detected carbon-containing products were generated from CO2under photocatalytic conditions. In situ diffuse reflectance infrared Fourier transform spectroscopy measurements further revealed the formation of carbonate, bicarbonate and hydrogenated carbon-containing intermediates during the reaction. This work offers a practical route for constructing metal–organic framework-derived Cu/TiO2photocatalysts for selective CH4production from CO2.
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Journal of Materials Chemistry A
·
2026
·
IF 9.2
Wenlong Yang,Zhenghui Ma,Guoli Fan,Xiaoyan Pu,Feng Li
Photocatalytic CO2 reduction to produce high value-added hydrocarbons has attracted significant attention, yet its overall efficiency remains unsatisfactory. In this work, a micro-liquid film reactor featuring enhanced mixing efficiency was utilized to realize the doping of single Fe atoms into the lattice of TiO2, enabling the generation of abundant atomically dispersed Feδ+ -Ov-Ti structures (Ov: oxygen vacancy). The results showed that compared to pristine TiO2, the optimized Fe-TiO2 photocatalyst bearing a 4 wt.% Fe content exhibited 15.2 times higher activity, with a significant shift in the predominant product from CO to CH4, as well as an impressively high CH4 formation rate of 29.2 μmol•g-1•h-1 , surpassing those over most of the state-of-the-art TiO2-based photocatalysts previously reported. It was revealed that the incorporation of single-atom Fe could reduce the bandgap of TiO2 matrix and surface atomically dispersed Feδ+ -Ov structures could improve the separation efficiency of photogenerated charge carriers and facilitated the adsorption and activation of CO2 and the formation and stabilization of key *CO reaction intermediate, thereby accelerating photocatalytic CO2 reduction to produce CH4. The present work affords a simple and efficient strategy for designing single-atom Fe-regulated TiO2-based photocatalysts for a synergistic enhancement of CO2 photoreduction activity and CH4 selectivity.
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