ACS Applied Materials & Interfaces
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2024
·
IF 8.3
Junwei Zhang,Kang Wang,Xitao Wang,Xingang Li
N-doped carbon materials have garnered extensive development in electrochemical CO2 reduction due to their abundant sources, high structural plasticity, and excellent catalytic performance. However, the use of powder carbon materials for electrocatalytic reactions limits their current density and mechanical strength, which pose challenges for industrial applications. In this study, we synthesized a monolithic N-doped carbon electrode with high mechanical strength for efficient electrochemical reduction of CO2 to CO through a simple pyrolysis method, using phenolic resin as the precursor and ZIF-8 as the sacrificial template. At 900 °C, the decomposition of ZIF-8 and the volatilization of Zn atoms promote the formation of a hierarchical porous structure in the carbon matrix, characterized by macropores with extended mesoporous channels. Simultaneously, N active species derived from ZIF-8 are effectively generated around the pores and fully exposed. The efficient mass transfer facilitated by the hierarchical porous structure and high activity of exposed nitrogen species enables efficient conversion of CO2 to CO. When the ZIF-8 content is 30%, the catalyst achieves a Faradaic efficiency of 88.9% for CO at a low potential of −0.7 V (vs RHE), with a CO production rate of 244.05 μmol h–1 cm–2. After 50 h of potentiostatic electrolysis, the current density and FECO remain stable. This work not only provides a strategy for the synergistic effects of hierarchical porous structures and nitrogen doping but also offers an effective method to avoid using powder binders and prepare integrated, stable monolithic electrodes.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Sisi Lin,Xinkui Wang,Xiaoyu Liang,Xinxin Zhang,Min Wang
Photocatalytic reduction of CO2 to high value-added chemicals and fuels has received widespread attention. However, the higher thermodynamic stability of CO2 greatly limits its conversion efficiency. Frustrated Lewis pairs (FLPs) have been well-established to be very effective in CO2 activation. In this work, we prepared ZnIn2S4–AlOOH (ZIS–AlOOH) composites for visible-light-driven CO2 reduction. The Lewis basic OHv sites on the AlOOH surface (one H removed from OH) and an adjacent Lewis acidic unsaturated Al site (Al3+unsatur.) form the FLPs. The composite structure facilitated light absorption, CO2 adsorption activation, and separation of photogenerated carriers, thus improving the CO2 photoreduction activity (CO generation rate of 510.3 μmol g−1 h−1), and suppressing hydrogen evolution with the CO/H2 ratio increasing from 0.38 for ZnIn2S4 (ZIS) to 0.84 for ZIS–AlOOH. This work elucidates a rational strategy for the construction of efficient photocatalysts and provides insight into the mechanism of the photocatalytic CO2 reduction reaction.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Guanhua Zhang,Shaocong Mo,Xiaowei Liao,Feng Liu,Hongtao Xu,Wei Lu
Metal-organic frameworks (MOFs) are interesting materials for carbon dioxide (CO 2 ) adsorption. Herein, novel nanocomposite materials comprising activated carbon (AC) and Magnesium-MOF-74 were synthesized by impregnating different loading ratios of activated carbon into synthesized Magnesium-MOF-74 to yield Magnesium-MOF-74@AC-X (where X represents the Magnesium/AC ratio set to 1:2, 1:1, and 2:1). Compared to Magnesium-MOF-74 alone, Magnesium-MOF-74@AC-X exhibited higher specific surface area, superior thermal stability, elevated CO2 adsorption capacity, and better adsorption selectivity. At 273 K, the adsorption of CO 2 by Magnesium-MOF-74@AC sample containing Magnesium to AC ratio of 1:2 reached 40.31 cm 3 /g, while that of pristine Magnesium-MOF-74 was only 21.01 cm 3 /g. At 298 K, the adsorption capacity reached 29.45 cm 3 /g, while that of pristine Magnesium-MOF-74 was 1.91-fold lower. The linear fitting of the adsorption isotherms of composite in the Henry adsorption region using Henry’s law yielded a CO 2 /N 2 selectivity adsorption capacity of 32.19, a value 4.55-fold higher than pristine Magnesium-MOF-74.
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ENVIRONMENTAL POLLUTION
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2024
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IF 7.6
Ruohua Qu,Na Liu,Qiong Wen,Jingyi Guo,Fei Ge
Algae-driven photosynthetic CO 2 fixation is a promising strategy to mitigate global climate changes and energy crises. Yet, the presence of metal nanoparticles (NPs), particularly dissolvable NPs, in aquatic ecosystems introduces new complexities due to their tendency to release metal ions that may perturb metabolic processes related to algal CO 2 fixation. This study selected six representative metal NPs (Fe 3 O 4 , ZnO, CuO, NiO, MgO, and Ag) to investigate their impacts on CO 2 fixation by algae ( Chlorella vulgaris ). We discovered an intriguing phenomenon that bivalent metal ions released from the metal NPs, especially from ZnO NPs, substituted Mg 2+ within the porphyrin ring. This interaction led to 81.8% and 76.1% increases in Zinc-chlorophyll and Magnesium-chlorophyll contents within algal cells at 0.01 mM ZnO NPs, respectively. Integrating metabolomics and transcriptomics analyses revealed that ZnO NPs mainly promoted the photosynthesis-antenna protein pathway, porphyrin and chlorophyll metabolism, and carbon fixation pathway, thereby mitigating the adverse effects of Zn 2+ substitution in light harvesting and energy transfer for CO 2 fixation. Ultimately, the genes encoding Rubisco large subunit ( rbcL ) responsible for CO 2 fixation were upregulated to 2.60-fold, resulting in a 76.3% increase in carbon fixation capacity. Similar upregulations of rbcL expression (1.13-fold) and carbon fixation capacity (76.1%) were observed in algal cells even at 0.001 mM ZnO NPs, accompanied by valuable lipid accumulation. This study offers novel insights into the molecular mechanism underlying NPs on CO 2 fixation by algae and potentially introduces strategies for global carbon sequestration.
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Qiong Liu,Chengbo Bai,Die He,Xueting Wu,Yiping Wu,Rong Chen
Surface defects in semiconductors play a significant role in modulating the performance of photocatalytic reactions. However, there is still insufficient exploration regarding the influence of defects on the photocatalytic CO 2 reduction performance. In this study, we achieved controllable construction of oxygen vacancies (OVs) in BiOX (X=Cl, Br) samples through one-step solvothermal treatment in polyols by adjusting the reaction time. The introduction of OVs significantly enhanced the photocatalytic activity of BiOX (X=Cl, Br) for converting CO 2 to CO. Among all the tested BiOX (X=Cl, Br) samples with OVs, BiOCl-OV-2 and BiOBr-OV-2 samples with a moderate amount of OVs exhibited the highest CO yield of 28.51 and 15.22 μmol g cat −1 after 4 hours of irradiation, respectively. Photo-/electrochemical measurements results revealed that engineering OVs into BiOX (X=Cl, Br) effectively adjusted their electronic structure, charge density and separation; however, excessive OVs may slightly degrade their photoelectrochemical properties and thus lead to reduced photocatalytic activity. Furthermore, an appropriate amount of OV was found to enhance both CO 2 adsorption capacity and photo-generated electron reduction ability, thereby further promoting the overall efficiency of photocatalytic CO 2 conversion. Through in situ FTIR spectra analysis, we uncovered the process of photocatalytic conversion from CO 2 to CO.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Yihui Li,Ziang Zhao,Min Zhao,Hejun Zhu,Xinzheng Ma,Zheng Li,Wei Lu,Xingkun Chen,Linbin Ying,Ronghe Lin,Yu Meng,Yuan Lyu,Li Yan,Yunjie Ding
Promotional effects of oxygen vacancies of spinel catalysts in CO 2 hydrogenation are reported in early works, but the mechanistic origins remain elusive. Here, CoAl 2 O 4 spinels with varying numbers of oxygen vacancies are deliberately designed by a sol-gel method and different post-treatments. By combining catalytic testing, advanced electron microscopic and spectroscopic characterizations, and computational studies, the unusual oxygen vacancy-dependent catalytic behaviors are rationalized. Our work reveals that i) perfect spinel crystals possessing least oxygen vacancies can effectively constrain the Co 2+ species at working conditions that are less active but selective to CO; and ii) vacancy-rich spinels promote both H 2 and CO 2 activations and COOH* formation, explaining the higher hydrogenation activity, but overwhelming vacancies cause Co 2+ reduction and promote direct CO 2 * dissociation to CO* and deep hydrogenation to CH 4 . These molecular-level understandings reinforce the idea of proper design of oxygen vacancies to achieve activity-selectivity balance.
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Molecular Catalysis
·
2024
·
IF 3.9
Yi He,Peng Bai,Shibo Yuan,Jiafa Chen,Yicheng Zhao,Yongdan Li
N -formylation of amines with CO 2 is a promising approach to high-efficient utilization of CO 2 as C1 feedstock, while conventional thermocatalytic processes suffer from harsh reaction condition and intense energy consumption. In this work, photocatalytic N -formylation of amines with CO 2 is achieved at room temperature over Pt-Bi/CeO 2− x composite catalyst. The Pt-Bi bimetallic sites increase the concentration of surface oxygen vacancies. Furthermore, the synergistic effects of Pt and Bi improve the light absorption capacity, reduce the band gap energy of the photocatalyst and promote the separation of photoinduced charge carriers. Using PhSiH 3 as the reducing agent, the conversion of N -methylaniline reaches 100 % after 3 h irradiation in N, N -dimethylformamide solvent with a N- methylformanilide selectivity of 90.8 %. The composite photocatalyst shows promising cycling stability and universality.
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Journal of CO2 Utilization
·
2024
·
IF 7.2
Luqman Abdullahi Sani,Haolong Bai,Zifu Xu,Liangliang Fu,Yining Sun,Xiaorui Huang,He Gao,Xuejing Liu,Dingrong Bai,Zhanguo Zhang,Fabing Su,Jiao Liu,Guangwen Xu
Ni/Al 2 O 3 catalysts (noted as Ni/Al-350, Ni/Al-500, and Ni/Al-700, respectively) were synthesized by a facile solution combustion method but at different combustion temperatures (350 °C, 500 °C, and 700 °C, respectively). For comparison, Ni/Al 2 O 3 (noted as Ni/Al-100) was also prepared by the impregnation method and applied in the methanation reaction. The Ni/Al 2 O 3 synthesized at the combustion temperature of 350 °C showed better performance than the others at higher combustion temperatures, and the activity for CO 2 methanation followed an order of Ni/Al-350 > Ni/Al-500 > Ni/Al-700 > Ni/Al-100. The increase in the combustion temperature decreased active sites for the H 2 and CO 2 adsorption, which could be associated with the reduced Ni dispersion and basic sites, thus lowering its activity and increasing its carbon deposition rate.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Keming Zhang,Sihui Li,Xiaohe Tian,Rui Zhang,Xiaoting Feng,Qingnan Wang,Yanting Tang,Chenlu Liu,Hongxia Gao,Shaofei Wang
Metal-organic framework (MOF) membranes demonstrate significant potential for industrial gas separations, yet fabricating vertically aligned two-dimensional (2D) MOF membranes on polymer substrates remains a considerable challenge due to the weak adhesion and difficulty in achieving precise alignment. This study presents a one-step method for the rapid synthesis of vertically aligned ZIF-L membranes, using a polydopamine (PDA)-assisted approach. This method enables the rapid formation of homogenous, thin but defect-free membranes on polymer substrates within 5 min, drastically reducing the preparation time by over 200 times. The vertically aligned ZIF-L membranes, characterized by the interlayer galleries facing the gas mixtures, exhibit an excellent CO 2 permeance exceeding 1200 GPU and a CO 2 /N 2 selectivity of 14.5. The versatility of this approach allows for its application on various flat-sheet or even hollow fiber supports. Our findings highlight the potential of PDA-assisted synthesis for efficient, scalable preparation of high-performance MOF membranes for industrial gas separations.
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Science Advances
·
2025
·Vol. 11
·期 12
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IF 12.5
Xiaoran Zhang,Yanhong Lyu,Jingjing Ding,Xin Wang,Bernt Johannessen,San Ping Jiang,Jianyun Zheng
l-phenylalanine (l-Phe), an essential amino acid for humans, is widely used as building blocks. Currently, l-Phe is obtained via biosynthetic methods including microbial and enzymatic processes, but their tightly complex feedback regulation and lengthy reaction steps lead to a low practical yield of l-Phe. Here, we have designed a hierarchical Si-based photocathode for l-Phe synthesis by photoelectrochemical coupling of waste CO2 and nitrophenyl ethane, achieving a high yield rate of 37.5 μg·hour−1·cm−2 and a remarkable Faradaic efficiency of 21.2% at low applied potential under 1 sun illumination. The hierarchical structure with CuO-TiO2-C mixtures dispersed in amorphous TiO2 layer/n+p-Si creates an internal built-in electric field and forms plentiful conducting channels to efficiently realize the injection of electrons into Cu and Ti sites. These Cu and Ti sites adsorb and activate the CO2 and nitrophenyl ethane, respectively, cooperatively facilitating the l-Phe synthesis. This work introduces an environmentally friendly and highly efficient approach for converting solar energy into valuable amino acid products.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xi Liu,Xueting Zhao,Zhiwen Lu,Kai Chen,Jiyuan Gao,Huibing Wang,Junxiang Chen,Zhenhai Wen
Amorphous electrocatalysts, unconstrained by crystalline order, offer a versatile landscape of active sites that promote enhanced reactivity and structural adaptability. When fused with the compositional complexity of high-entropy materials, this disordered architecture yields enhanced electronic interactions and catalytic adaptability. In this work, we design a self-supporting amorphous high-entropy oxide (a-HEO) electrode by in-situ growth of FeCoNiMnMo-based nanosheets on nickel foam (a-FeCoNiMnMoO/NF). Electrochemical activation triggers a self-reconstruction process, yielding oxyhydroxide species embedded with oxygen vacancies that collectively enhance electron conductivity and catalytic performance for the alkaline methanol oxidation reaction (MOR). Machine learning potential-based simulations demonstrate that the amorphous oxyhydroxide layer offers a diverse array of catalytic sites, fine-tunes the electronic structure, and optimizes intermediates adsorption, thus enhancing the reaction dynamics of methanol oxidation. When employed in a hybrid acid/alkali flow electrolyzer, the system operates at just 0.54 V to reach 10 mA cm −2 , enabling over 300 h of continuous, CO 2 -free production of hydrogen and formate, demonstrating a durable and energy-saving strategy for sustainable fuel and chemical generation. This study highlights the compelling synergy between structural disorder and elemental complexity, charting a promising course toward low-energy, carbon-neutral methanol reforming and sustainable hydrogen production.
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RSC Advances
·
2024
·Vol. 14
·期 10
·6502-6507
·
IF 3.9
Jiaqi Wang,Kaihong Liu,Jingjing Zhao,Xiuping Li,Bolin Yin,Bo Jiang,Hexing Li
Direct CO2 hydrogenation to value-added chemicals is a promising path toward realizing the “carbon-neutral” goal. However, controlling the selectivity of CO2 hydrogenation toward desired products (e.g., CO and CH4) using non-precious metal-based catalysts is important but challenging. It is imperative to explore catalysts with high activity and stability. Herein, boron-doped cobalt nanoparticles supported on H-ZSM-5 were devised for CO2 hydrogenation to produce CO in a gas–solid flow system. Our results demonstrate that boron doping not only increases the CO2 adsorption capability of the catalyst but also optimizes the electronic state of Co for CO desorption during hydrogenation process. As a result, the boron-doped cobalt catalysts displayed an enhanced CO selectivity of 94.5% and a CO2 conversion rate of 45.6%, which is much higher than that of Co-ZSM-5 without boron doping. This study shows that the strategic design of metal borides is important for controlling the selectivity of desired products in the CO2 hydrogenation reaction.
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