CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Cong Wan,Jianwen Zhang,Honglei Zhang,Min Liu,Yiming Li,Zijun Yan,Chengheng Pang,Tao Wu
The catalytic reduction of CO₂ into valuable chemicals and fuels is a promising strategy for mitigating global carbon emissions. This study explores the synergistic co-reduction of CO₂ and H₂O using nanoscale zero-valent iron (NZVI) as a dual-function catalyst. Under light irradiation at 300 °C, the CO₂ reduction rate increased by more than 10-fold compared to dark conditions, demonstrating significant photothermal synergy. The study reveals that NZVI undergoes a phase transformation, where Fe₃O₄ functions as a photocatalyst while Fe 0 serves as an electron donor, enabling a unique dual-functionality that facilitates efficient electron transfer. The addition of 10 vol% H₂ stabilizes the reaction, leading to a higher and more consistent CO yield. When investigating the simultaneous reduction of CO₂ and H₂O, we discovered competitive adsorption and reaction pathways that significantly influence product distribution. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations revealed three distinct mechanistic pathways for CO₂ conversion: direct C O bond cleavage, a carboxylate-mediated pathway and bicarbonate-mediated pathway, with the carboxylate and bicarbonate pathways being uniquely promoted by H and OH from H₂O dissociation. The addition of H₂O into the CO₂ and H₂ reaction significantly enhanced CH₄ generation due to the extra H source from H₂O dissociation. These findings offer valuable insights into the competitive mechanistic pathways of CO₂-H₂O co-reduction and contribute to the design of more efficient iron-based catalysts for sustainable CO₂ conversion and water splitting in energy and environmental applications.
研究领域:
环境催化
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纳米科技
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可再生能源
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表面化学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
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2024
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IF 6.7
Yiming Chen,Chuan Wang,Qianwen Zhang,Ling Zhou,Yi Zhang
Methane synthesis derived from CO 2 hydrogenation has attracted great attention in terms of CO 2 recycling while suffering from the loss and sintering of active nickel species. Hence, we synthesized the Ni@Beta (Si/Al = 40) catalyst with a specific encapsulated structure by a simple hydrothermal synthesis using conventional Ni/SiO 2 as a unique silicon source. Compared to the conventional Ni/SiO 2 and Ni/Al 2 O 3 , the Ni@Silicalite-1 and Ni@Beta with encapsulated structures showed better stability. In addition, the Ni@Beta simultaneously exhibited the highest CO 2 conversion (74.2 %) and methane selectivity (93.5 %). All obtained catalysts were characterized by BET, ICP- OES, XRD, SEM-EDS, HRTEM, H 2 -TPR, CO 2 -TPD, in situ XPS, in situ DRIFTS, and NAP-XPS. Compared with the Ni@Silicalite-1 (Al-free zeolite), the aluminum-containing zeolite frameworks of the Ni@Beta got more electrons from the nickel active phases, so the metal-support interaction on the Ni@Beta was stronger, which was favorable for the stability of the Ni 0 phase. In addition, the Al-containing zeolite frameworks of the Ni@Beta inhibited the formation of volatile metal–molecule intermediates (gaseous Ni(CO) x ), which prevented serious sintering and loss of the nickel species. The in situ DRIFTS and NAP-XPS results not only successfully unveiled that the main reaction pathway was a formate route, but also showed that the Ni@Beta had the strongest capacity to adsorb and convert CO 2 , so it had the highest methanation activity.
研究领域:
催化
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化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Xing Yan,Dongren Cai,Meihong Lin,Zhijie Wu,Yegang Xia,Yanmei Cai,Sajid Ali,Kok Bing Tan,Andriambinintsoa Ranaivoson Tojonirina,Hao Sun,Guowu Zhan
The selective hydrogenation of CO 2 to methanol demands precise control of both catalyst architecture and reaction pathways. Here, we design an atomic layer deposition (ALD)-engineered Pd/ZnO/ZrO 2 ternary catalyst with atomic-scale ZnO interlayers to decouple and reconfigure active sites at dual interfaces (Pd-ZnO and ZnO-ZrO 2 ). This interfacial engineering drives a 7-fold enhancement in methanol space–time yield (0.584 vs. 0.084 g MeOH g cat −1 h −1 ) and switches the dominant reaction pathway from CO-mediated to formate-driven selectivity (methanol selectivity remarkably surges from 6 % to 64 %). Multimodal characterization and theoretical calculations reveal that ZnO interlayers orchestrate bifunctional cooperation: activating CO 2 /CO adsorption while suppressing CO/CH 4 formation through electronic effects. Long-term stability study uncovers a dynamic restructuring mechanism, where Pd-ZnO interfaces gradually evolve into PdZn β alloy phases under the reaction conditions. This work establishes ALD-mediated interface design as a generalizable strategy to manipulate reaction networks and methanol selectivity in catalytic CO 2 hydrogenation systems.
研究领域:
催化化学
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材料科学
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化学工程
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可持续能源
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
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2025
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IF 10
Lehang Liang,Weixin Kong,Zhiyuan Dong,Xinling Zhong,Tao Song,Tao Wang,Mengxiang Fang,Wei Li,Sujing Li
Chemical absorption using amine blends is a viable strategy for energy-efficient post-combustion CO 2 capture. Conventional amines suffer from high regeneration energy due to carbamate formation, whereas bicarbonate pathways offer thermodynamic benefits yet remain mechanistically unresolved. Herein, we developed a novel aqueous ternary amine blend, APH (7.5 wt% 2-amino-2-methyl-1-propanol, AMP/7.5 wt% piperazine, PZ/15 wt% 4-hydroxy-1-methylpiperidine, HMPD) that leverages molecular synergy to shift CO 2 absorption toward bicarbonate dominance. APH achieved absorption rate of 30 wt% MEA (0.00206 mol⋅min −1 ) while exhibiting a 175 % higher stabilized cyclic capacity (0.553 mol⋅mol −1 ) over five regeneration cycles. Combined 13 C NMR and DFT analyses revealed three synergistic bicarbonate-forming pathways: steric hindrance-induced carbamate hydrolysis, promoter-derived stepwise carbamate hydrolysis, and tertiary amine-catalyzed CO 2 hydration. Optimized AMP/PZ/HMPD ratios delivered 41 % lower regeneration energy (2.32 GJ⋅t −1 CO 2 ), low corrosion (0.0358 mmpy), and enhanced oxidative stability (88 % retention after 14 days). These advances stem from a molecular design approach correlating structural features with intermolecular synergies for pathway modulation. The APH blend thus emerges as a promising candidate for industrial applications.
研究领域:
化学工程
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环境科学
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材料科学
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物理化学
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工业化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
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2024
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IF 3.7
Zihan Yu,Jun Mao,Qiong Li,Yuanyuan Hu,Zhanlong Tan,Fei Xue,Yonglian Zhang,Hongxiang Zhu,Chunfang Wang,Hui He
To ensure prolonged functionality of transpiration-driven electrokinetic power generators (TEPGs) in saltwater environments, it is imperative to mitigate salt accumulation. This study presents a salt pathway transpiration-driven electrokinetic power generator (SPTEPG), incorporating MXene, graphene oxide (GO), and carbon nanotubes (CNTs) as active materials, along with cellulose nanofibers (CNF) and poly(vinyl alcohol) (PVA) as aqueous binders and nonwoven fabrics. This unique combination confers exceptional hydrophilicity and enhances the energy generation performance. When tested with deionized water, the SPTEPG achieved a maximum voltage of 0.6 V and a current of 4.2 μA. In simulated seawater conditions, the presence of conductive ions in the solution boosted these values to 0.64 V and 42 μA. The incorporation of the salt pathway mechanism facilitates the return of excess salt deposits to the bulk solution, thus extending the SPTEPG’s service life in saltwater environments. This research offers a straightforward yet effective strategy for designing transpiration-driven power generators suitable for saline water applications.
研究领域:
材料科学
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电化学
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可再生能源
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）