Frontiers in Energy Research
·
2023
·
IF 3.4
Huang Jiamin,Zhang Guanghui,Wang Mingrui,Zhu Jie,Ding Fanshu,Song Chunshan,Guo Xinwen
The catalytic production of higher alcohols (HAs) is a promising path for converting CO2 into value-added chemical products. The application is still limited by the low selectivity of HAs (less than 10%) on most catalysts. Here, we report a tandem catalyst consisting of Mn-Cu-K modified iron carbide and CuZnAlZr catalyst. The modification of iron carbide with Mn, Cu and K promoters improves the formation of HAs (13.5% Sel.), and the construction of tandem catalysts with CuZnAlZr can further enhance the catalytic performance. By examining different catalyst filling methods and the filling ratio of the tandem catalyst, it was found that the powder mixing resulted in a higher selectivity of HAs with a mass ratio of the two components of 1:1, and a synergistic effect leads to a higher selectivity of HAs (15.5%) with about 40% of propanol and butanol among HAs.
研究领域:
化学工程
·
催化科学
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高影响因子
Nature Communications
·
2026
·
IF 18.1
Li Ling,Ning Shangbo,Cheng Fangqi,Chen Mingjun,San Xingyuan,Hu Zhuofeng,Gao Linjie,Tang Yuan,Hao Yuchen,Lv Cuncai,Li Yaguang,Ye Jinhua
Photothermal hydrogenation of CO 2 offers a solar-driven route to multicarbon hydrocarbons, but controlling carbide formation and maintaining reconstructed active sites remain challenging for iron-based catalysts. Here, we develop a trace Al/Rb co-promoted CuFe 2 O 4 catalyst that enables efficient and stable photothermal CO 2 hydrogenation to light olefin under ambient pressure. The optimized catalyst achieves high C 2 -C 4 olefin selectivity of approximately 63%, suppressing CH 4 selectivity and sustaining stable photothermal-catalytic performance for 200 h. Integrated experimental characterizations and theoretical calculations reveal that the CuFe 2 O 4 precursor undergoes reaction-induced reconstruction to form Cu-Fe 5 C 2 interfacial structures. Trace Al/Rb promotion facilitates the formation and stabilization of reconstructed metal–carbide interfaces, with Al regulating the Fe-centered coordination environment and carbide stability, while Rb tunes the interfacial electronic structure and adsorption–hydrogenation balance. This cooperative regulation stabilizes carbide-based interfacial active sites and promotes CO 2 -derived C 1 intermediates toward C–C coupling and C 2 -intermediate stabilization, thereby favoring C 2 -C 4 olefin formation.
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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Yuan Li,Ruizhe Li,Pingping Rui,Jingwen Cheng,Yunxiang Li,Hong Yuan,Shuxin Ouyang
Fischer–Tropsch synthesis (FTS) offers a route for converting syngas from nonpetroleum resources into valuable chemicals, such as light olefins. χ-iron carbide (χ-Fe5C2), the key active phase for olefin production, is plagued by poor stability under practical conditions. Here, we propose a synthesis-to-catalysis full-process Cu-assisted strategy that integrates synthesis, photothermal conversion and reaction regulation into a design framework, thereby enabling a Cu/Fe5C2@C catalyst with improved durability and catalytic performance. The optimized 0.20Cu/Fe5C2@C catalyst achieves 48.7% light olefins selectivity, a 3.1-fold increase in light olefin yield compared to Fe5C2@C, and markedly improved long-term stability under photothermocatalytic FTS. Mechanistic studies reveal that the full-process synergy of Cu enhances catalytic performance by promoting the formation of a highly graphitized carbon shell to stabilize χ-Fe5C2 during synthesis, enhancing photothermal conversion efficiency via localized surface plasmon resonance, and optimizing reactant activation and the CH2* intermediate transformation toward light olefins. This work establishes a full-process regulation paradigm that integrates multistage functions, offering a transformative approach toward high-performance, durable solar-driven FTS for nonpetroleum resource utilization.
研究领域:
催化化学
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材料科学
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能源化学
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纳米技术
·
可持续能源
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Fang Li,Wenjie Cui,Jiangyong Liu,Yongping Zeng,Xue Ye,Jie Li
Achieving high selectivity to light olefins from CO2 hydrogenation under ambient pressure remains challenging due to unfavorable phase dynamics and excessive RWGS activity in iron-based catalysts. Comprehensive characterization reveals that moderate Ca addition inhibits water-induced oxidation of Fe5C2, stabilizes carbide phases, promotes electron transfer from CaCO3 to Fe species, and enhances CO transferfrom Fe3O4 (RWGS sites) to Fe5C2 (FTS sites). These effects synergistically suppress CO and CH4 formation while facilitating C–C coupling. The optimized Ca8K8FeMn catalyst delivers 26.9% CO2 conversion, 68.6% CO selectivity, 59.3% light olefins selectivity in hydrocarbons, and a space-time yield of 33.5 gC2‐C4=kgcat‐1h‐1 at 320 °C, 0.1 MPa, H2/CO2 = 3, GHSV = 3600 mL·g–1·h–1. Compared to the unmodified K8FeMn, CO selectivity decreases by ∼30%, CH4 by ∼10%, light olefins selectivity increases by 7.7%, and STY improves 6-fold. This work elucidates the critical roles of phase equilibrium and electronic modulation in ambient-pressure CO2-to-olefins catalysis.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 29
·15459-15472
·
IF 3.9
Li Xiaolong,Zhang Yahui,Sun Gangqun,Sun Manni,Wang Xiru,Yang Zhiyan,Zhao Zhuoya,Li Mengjie,Ma Yongning,Huang Wei,Zhu Junli,Yang Yuhao
The
development of high-performance catalysts enabling CO-free
hydrogen production via aqueous-phase reforming of methanol (APRM)
is crucial for integrated methanol-to-hydrogen and hydrogen fuel cell
systems. Herein, a tandem Pt/Fe 5 C 2 :Fe 3 N@C catalyst was prepared via a temperature-programmed carbonization-nitridation
method followed by photoreduction deposition. Remarkably, the catalyst
delivers efficient CO-free H 2 production even at temperatures
as high as 210 ° C. The catalyst features a strong metal–support
interaction between Pt and Fe 5 C 2 , and a weaker
interaction between Pt and Fe 3 N. Mechanistic investigations
decouple the functions of the individual components. The carbon support
primarily serves to disperse the active components. The Pt–Fe
interface provides the active sites for methanol decomposition (CH 3 OH → CO + 2H 2 ). The resulting CO is completely
consumed through two subsequent reactions: most undergoes the water–gas
shift reaction (CO + H 2 O → CO 2 + H 2 ) on the surfaces of Fe 3 N and Fe 5 C 2 , with Fe 3 N being the dominant active phase, while
the remaining trace CO undergoes methanation (CO + 3H 2 →
CH 4 + H 2 O), for which Fe 5 C 2 is the principal active site. This synergistic cascade of reactions
enables the Pt/Fe 5 C 2 :Fe 3 N@C catalyst
to achieve highly efficient CO-free hydrogen production from APRM.
This work offers insights into designing catalysts for CO-free hydrogen
generation from alcohol-based liquid organic hydrogen carriers and
may accelerate the integrated industrialization of the methanol-to-hydrogen
and hydrogen fuel cell technology.
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高影响因子
FUEL
·
2022
·
IF 8.035
Zhunzhun Ma,Weixin Qian,Haitao Zhang,Hongfang Ma,Qiwen Sun,Weiyong Ying
Fischer–Tropsch-to-Olefins (FTO) over iron-based catalysts is a promising process for the production of light olefins from a non-petroleum source. However, the catalytic mechanism is unclear because of the variation in the iron phase during the reduction and activation processes and the complex iron phase composition under the reaction conditions. A series of Li-promoted FeMnMgO x catalysts is synthesized using co-precipitation and impregnation methods, after which the effect of promoters on the evolution of the iron phase, chemisorption, and FTO performance are analyzed. The results demonstrate that Mg enhances dissociative CO adsorption and hydrogen adsorption, improving the FTO activity. Mg facilitates the dispersion of α-Fe 2 O 3 and suppresses the carbonization , which weakens the chain propagation, encourages the formation of short-chain hydrocarbons, and increases the selectivity of light olefins . Li also enhances dissociative CO adsorption and increases CO conversion. Moreover, Li facilitates the formation of the ε'-Fe 2.2 C phase, which reveals a higher FTS activity and better C–C coupling ability than the χ-Fe 5 C 2 phase. This results in a decrease in CO 2 and increase in light olefins . At the optimal Li loading, the FeMnMg-0.75Li sample displays the highest space time yield of light olefins at 355 g/(kg cat ·h).
研究领域:
化学工程
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催化
·
材料科学
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高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Minjie Xu,Xianglin Liu,Guiyao Song,Yingying Cai,Bianfang Shi,Yitao Liu,Xiaoxu Ding,Zixu Yang,Pengfei Tian,Chenxi Cao,Jing Xu
Different iron species exhibit distinct activity and selectivity in CO 2 hydrogenation reaction. Herein, by controlling calcination temperature, Fe-Al interaction in Na promoted Fe-Al catalysts has been regulated, which further leads to various compositions of iron oxide (FeO x ) and iron carbides (Fe 7 C 3 and Fe 5 C 2 ) after CO activation and CO 2 hydrogenation reaction. The phase compositions and structures of Fe-Al catalysts are carefully distinguished by multiple characterizations, including XRD, XPS, MES and TEM, and the reactivity of different phases is studied with the combination of experiments (kinetics, TP and in situ DRIFTS) and Density Functional Theory (DFT) calculations. Our FeAl350 with the highest FeC x content shows the highest CO 2 conversion of 48.2% and the lowest CO selectivity of 10.1%, and FeAl900 with the highest Fe 5 C 2 / FeC x ratio presents the highest C 5+ selectivity of 44.6%. Finally, a correlation between different compositions of iron species with the activity and selectivity of Fe-based for CO 2 hydrogenation to olefins was established.
研究领域:
催化
·
化学工程
·
材料科学
·
环境化学
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产品关联
DOI
高影响因子
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