Materials Today Energy
·
2023
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IF 9.3
Fangyuan Zhang,Xueli Zhang,Shan Hu,Huilin Hu,Jinhua Ye,Defa Wang
Photothermal catalytic carbon dioxide (CO 2 ) reduction has attracted increasing research attention as a promising method for recycling CO 2 and producing renewable energy. However, it remains a challenge in the improvement of catalytic activity with regulated product selectivity in view of practical applications. Herein, we develop the two-dimensional layered V 2 C MXene (VC) supported Ni nanoparticle and NiO nanosheet (Ni@NiO/VC) composite as an efficient catalyst for selective photothermal reduction of CO 2 to CH 4 . The optimal 0.8Ni@NiO/VC catalyst exhibits 48.1 % CO 2 conversion with an evolution rate of 33.2 mmol/g cat /h and 99.2 % selectivity for CH 4 production under a 300 W full-arc xenon lamp irradiation. Moreover, a long-term cyclic photothermal CO 2 reduction reaction demonstrates the excellent stability of 0.8Ni@NiO/VC. The enhanced photothermal CO 2 reduction activity with a high CH 4 selectivity could be attributed to the large specific surface area and excellent photothermal effect of V 2 C MXene, and the synergistic effect of Ni and NiO on adsorption/activation of H 2 and CO 2 molecules. This work provides a feasible strategy for the construction of efficient photothermal CO 2 reduction catalyst by properly incorporating transition metal nanoparticles and metal oxide with a suitable MXene.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
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IF 9.5
Ke Chen,Linhan Ni,Xin Guo,Chengming Xiao,Yue Yang,Yujun Zhou,Zhigao Zhu,Junwen Qi,Jiansheng Li
The performance of mixed matrix membranes (MMMs) substantively depends on the intrinsic structure and composition of the introduced nanofillers. In this work, pyrazole-based metal-organic frameworks (termed as MOF-303) were introduced into polymer of intrinsic microporosity (PIM-1) through a physical blending approach. Thanks to the well CO 2 -philic capability, high porosity, and appropriate pore structure of the incorporated MOF-303, the obtained MMMs exhibited remarkable separation performance. The improved CO 2 permeability and well-maintained CO 2 /CH 4 selectivity were achieved. Specifically, MMMs introducing 30 wt% MOF-303 loading exhibited a CO 2 /CH 4 selectivity of 27.6 and a high-CO 2 permeability of 7528.2 Barrer, which were 2.2 and 1.9 times greater than those of the unfilled PIM-1 membranes, respectively. Furthermore, a 33-h continuous separation test verified the excellent stability of the manufactured MMMs. More importantly, the MMMs showed significant resistance against physical aging, retaining up to 92.8% of their original CO 2 permeability after 150 days, compared to just 33.0% for control PIM-1 over the same period. Meanwhile, the plasticization resistance of the MMMs was reinforced compared to the unfilled PIM-1 membrane. This study potentially provides a novel approach for the rational design of MMMs in CO 2 separation applications.
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Solar RRL
·
2021
·Vol. 5
·期 4
·2000813
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IF 8.582
Di Li,Changjian Zhou,Zhongkai Xie,Donghai Chen,Yimeng Zhou,Xiangli Shi,Deli Jiang,Min Chen,Weidong Shi
Due to the low charge separation efficiency and high stability of the CO 2 molecule, photoreduction of CO 2 into a single multielectron product such as CH 4 with a simultaneous high conversion rate and selectivity is challenging. Therefore, it is highly desirable to accelerate charge separation and transfer and provide an electron-enriched catalyst surface for the deep reduction of CO 2 . Herein, a Pd/Cu 2 O/TiO 2 ternary hybrid photocatalyst consisting of Pd nanoparticles (NPs) and Cu 2 O NPs-decorated TiO 2 nanosheets is rationally designed, and highly selective photocatalytic photoreduction of CO 2 into CH 4 is achieved. The Pd/Cu 2 O/TiO 2 photocatalyst shows a high CH 4 production rate of 42.8 μmol g −1 h −1 with an extremely high selectivity of 99.5%. This CH 4 production rate is 61.1, 5.4, and 2.8 times higher than the bare TiO 2 , Cu 2 O/TiO 2 , and Pd/TiO 2 , respectively. In this Pd/Cu 2 O/TiO 2 hybrid, a consecutive multistep charge transfer is steered between the Cu 2 O/TiO 2 heterojunction and Pd, ensures accelerated charge separation and transfer, and leads to the formation of a spatially separated electron-enriched surface (Pd) and hole-enriched surface (Cu 2 O). This spatially oriented charge transfer and the charge-enriched catalyst surface synergistically contribute to the simultaneous high conversion rate and selectivity of CH 4 .
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FUEL
·
2021
·
IF 6.609
Pengfei Cao,Haitao Zhao,Stephen Adegbite,Bolun Yang,Edward Lester,Tao Wu
CO 2 dry reforming of methane (DRM) is one of the most promising routes for the large-scale utilization of greenhouse gases (CO 2 and CH 4 ). However, it is still of challenges to develop catalysts that are efficient and cheap but are of high resistivity in coke formation to maintain long-term stability. Herein, K 2 CO 3 was used as a promoter to enable dynamic coke elimination reaction over the Ni/Al 2 O 3 for CO 2 reforming of CH 4 . K 2 CO 3 -modified Ni/Al 2 O 3 catalysts were synthesized via a wet co-impregnation method and investigated for DRM. The 1.0 K-Ni/Al 2 O 3 exhibited the best stability in the test of 96 h on stream at 800 °C. It was found that coke resistance of K 2 CO 3 modified catalyst was significantly improved, as the coke formation on 1.0 K-Ni/Al 2 O 3 catalyst was only 1/3 of that on Ni/Al 2 O 3 catalyst after a long-term test. Characterization results showed that the growth of Ni particles was suppressed because the addition of K 2 CO 3 enhanced the interaction between Ni and Al 2 O 3 . Meanwhile, the addition of K 2 CO 3 raises the basicity of the catalysts, which enhances the adsorption of CO 2 on the surface and subsequently facilitates CO 2 dry reforming of CH 4 . In addition, the transient experiment reveals that K 2 CO 3 enables a dynamic coke elimination reaction (KCER) via enhancing the catalytic reaction of disordered carbon with CO 2 , which is considered as a promising low-cost approach to stabilize the performance of the Ni-based catalysts in DRM reaction.
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CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Zhongliang Huang,Yujia Yuan,Miaomiao Song,Zhimian Hao,Jingran Xiao,Dongren Cai,Abdul-Rauf Ibrahim,Guowu Zhan
Herein, we fabricated a series of bimetallic Pt-Ni catalysts supported on mesoporous silica nanorods ( m SNR, specific BET surface area of 1802 m 2 g −1 ) to study the effect of Ni/Pt ratio on the product selectivity in CO 2 hydrogenation. Both monometallic Pt/ m SNR and Ni 50 Pt 50 / m SNR catalysts revealed negligible methane selectivity. However, methane became the major product only when increasing the Ni/Pt ratio up to 9. X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma (ICP) characterizations showed that the Pt/Ni ratio on the catalyst surface was appreciably higher than the bulk composition, suggesting the enrichment of Pt on the surface ( e.g. , Pt/Ni of 61/39 for Ni 50 Pt 50 / m SNR catalyst). The Pt/Ni ratio was crucial in determining the CH 4 /CO selectivity, and the addition of a tiny amount of Pt could improve the catalytic performance and stability of Ni/ m SNR. Among the different catalysts, Ni 98 Pt 2 / m SNR showed the best CO 2 conversion (59%) and CH 4 selectivity (96%) at 400 °C, 0.1 MPa, 9600 mL h −1 g cat −1 , and H 2 /CO 2 of 3. In-situ DRIFTS and temperature-programmed surface experiments suggested that the dissociated adsorption of CO 2 on the Pt site led to CO*, but the strongly adsorbed CO* cannot be further hydrogenated to CH 4 over the Pt site. In contrast, CO* could be further hydrogenated into CH 4 via CH x O* intermediates on adjacent Ni sites.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Xiaodi Zhang,Guojie Zhang,Xiaowei Qin,Jun Liu,Guoqiang Li,Ying Xu,Yongkang Lv
A series of nitrogen doped biomass carbon catalysts were prepared through two different nitrogen doped methods by using soybean meal as the raw material, melamine as nitrogen source and KOH as the activators. The catalysts were characterized by BET, SEM , CO 2 -TPD, EA , FTIR , XPS and Raman. The catalytic performances of CH 4 –CO 2 reforming over different samples were also studied. The results show that the preparation method of the catalyst significantly affects the structural characteristics, N content and N species type of the catalyst. The characterization results also show the proportion of pyrrolic-N in the catalyst prepared by in-situ nitrogen doped method (Y-NC) is higher than that in prepared by the post-treatment method (H-NC). Pyrrole-N is more conducive to the adsorption and activation of CO 2 . So, the catalyst prepared by in-situ nitrogen doped method has good catalytic activity and stability. The conversion of CH 4 and CO 2 were respectively 40% and 65% at 900 °C after 50 h of CH 4 –CO 2 reforming reaction .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Sheng Li,Guojie Zhang,Jiming Wang,Jun Liu,Yongkang Lv
Carbon materials are widely used as catalysts or supports due to their excellent properties. In this paper, the tungsten carbide-activated carbon (WC-AC) composite support was successfully prepared by in-situ carburizing on AC matrix, which is characterized by the covalent anchoring of WC on the AC support. The active metal Co was supported on WC-AC for dry reforming of methane (DRM). Samples were analyzed by N 2 physisorption measurements, XRD , XPS , H 2 -TPR, H 2 -TPD, CH 4 &CO 2 -TPSR, TG-DTG. The WC-AC stabilizes the disturbance of C in AC, alleviates the gasification effect of CO 2 and increases the active sites for CH 4 cracking. Moreover, WC provides a resistance-less bridge suitable for the Co 3+ → Co 2+ , resulting in a high Co 2+ /Co 3+ ratio on the catalyst surface . This enhances the interaction between the Co species and the WC-AC, thereby enhancing the CH 4 activation. In the process of WC-AC promoting Co 3+ →Co 2+ , the catalyst surface is accompanied by the generation of oxygen vacancies . This can enhance the dissociative adsorption of CO 2 on surface of the WC-cobalt oxide, and at the same time increase the relative proportion of adsorbed oxygen on the catalyst surface, thereby effectively inhibiting the formation of coke. However, the small amount of graphitic carbon generated due to the strong coupling of WC and Co is the main reason for deactivation of Co/WC-AC.
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CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Daofei Lv,JiaYu Chen,Kexin Yang,Houxiao Wu,Yongwei Chen,Chongxiong Duan,Ying Wu,Jing Xiao,Hongxia Xi,Zhong Li,Qibin Xia
Using porous materials to selectively adsorb CO 2 from flue gas or natural gas is a promising method for mitigating CO 2 emission and purifying methane. Here, we synthesized an L-aspartic acid based microporous metal-organic framework (MIP-202) and studied its adsorptive separation performance for CO 2 /CH 4 and CO 2 /N 2 mixtures. Results show that MIP-202 had ultrahigh CO 2 /CH 4 (72.9 and 241.5 for CO 2 /CH 4 = 50/50 and 10/90, respectively) and CO 2 /N 2 (1,950,000 and 2129.1 for CO 2 /N 2 = 50/50 and 15/85, respectively) IAST selectivities at 298 K and 100 kPa. The high selectivity was verified by the calculations of Henery’s law selectivity and breakthrough experiments. Metropolis Monte Carlo simulation calculations show that CO 2 with greater polarizability and quadruple moment tends to occupy the pore walls of large cages with higher polarity, while the less polar CH 4 or N 2 majorly being adsorbed in the pore walls of small cages with lower polarity, resulting in the ultrahigh CO 2 /CH 4 and CO 2 /N 2 separation selectivities. MIP-202 exhibits low CO 2 adsorption enthalpy (17.2–30.7 kJ/mol), superior persistent reusability after five cyclic adsorption experiments, easy desorption performance at 298 K, moderate water and moisture stability, good stability under dry and humid SO 2 atmosphere, and low ligand cost ($36/kg). MIP-202 extrudates were prepared by an extrusion molding method using hydroxypropyl cellulose (HPC) as the binder and they retained 97.35% CO 2 uptake of MIP-202 powder at room temperature and pressure. This work shows that MIP-202 is an industrially promising material for the separation of CO 2 /CH 4 and CO 2 /N 2 mixtures.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2015
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IF 2.037
Qiaobei Dong,Yan Sun,Wei Su,Jia Liu
The use of hydrate formation in porous media is an effective method for gas storage and separation. The equilibrium isotherms of CH4 and N2 in CMK-3, a mesoporous carbon material, were measured under different tetrahydrofuran (THF) concentrations and temperatures. The higher is the temperature required, the greater is the formation pressure needed, but the presence of THF significantly reduces the hydrate formation pressure. When THF exists, both CH4 and N2 form structure II (sII) hydrate; however, the amount of hydrate generation is lower than the theoretical value. As the operating pressure increases, some of the sII CH4 hydrate may transform into structure I (sI) and the amount of hydrate generation increases. The desorption isotherms showed that the gas hydrate decomposed completely when the operating pressure was below the hydrate decomposition pressure. In addition, it is feasible to separate gas mixtures via hydrate formation using the different gas hydrate formation pressures.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Run-Jing You,Kuan Wang,Huan Ma,Xin-Peng Li,Zhe Cao,Zhen-Hong He,Huan Wang,Weitao Wang,Xiaojuan Lai,Zhao-Tie Liu
The utilization of solar energy in photocatalytic CO 2 reduction technology has demonstrated a significant potential in addressing the challenges of environmental pollution and energy shortage issues. Precise modulating of the photoreduction CO 2 pathway to achieve desired products is of particular interest, while the design of cost-effective and robust catalysts remains crucial. Herein, a series of BiOBr-based photocatalysts with different Co species were synthesized through a facile simple hydrothermal method in combination with the mechanical mixing. The Co species, which can be precisely modulated from Co 3 O 4 to CoOOH by adjusting the concentration of H 2 O 2 , were anchored into the BiOBr nanospheres to establish rich Z-scheme heterojunction interfaces. The Co species modulating of BiOBr-based Z-scheme heterojunction can achieve the transform photoreduction CO 2 products from CO to CH 4 . The CO selectivity in CO 2 photoreduction to reached 98.10 % (54.10 μmol·g −1 ·h −1 ), while the CH 4 selectivity over CoOOH/BiOBr reached 72.59 % (20.06 μmol·g −1 ·h −1 ). The outstanding photocatalytic performance and selective regulation of products are ascribed to the modulation of Co species in the BiOBr-based heterojunctions, which enables the customization of the photoreduction CO 2 pathway to achieve the desired products transformation from CO to CH 4 . In situ experiments and theoretical calculations reveal that the excellent CO selectivity observed in Co 3 O 4 /BiOBr heterojunction can be ascribed to a lower energy for *CO species compared with that of hydrogenation to *HCOOH and *CHO intermediates. Conversely, the presence of *HCOOH and *CHO intermediates with lower energy levels compared with *CO species achieved superior CH 4 selectivity in CoOOH/BiOBr heterojunction. This precise design strategy insights into the meticulous customization of Co species in semiconductor-based heterostructures at the molecular level, and enlightens the selective regulation of desired products for catalysis applications.
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Molecular Catalysis
·
2024
·
IF 3.9
Yinan Ren,Wei Li
Solar-driven CO 2 reduction into hydrocarbon fuels has a great potential for mitigating the issues of greenhouse effect and fossil energy crisis we are currently facing. It is a great challenge for visible-light-driven photocatalytic CO 2 reduction into CH 4 with high selectivity and conversion efficiency. Herein, we report a synthesis of N/K-doped TiO 2 nanospheres with Ag nanoparticles decoration (N/K-TiO 2 -Ag) by a solvothermal method and study its photocatalytic CO 2 reduction performance. It is found that the N/K-TiO 2 -Ag composite exhibits superior photocatalytic CO 2 reduction into CH 4 yield and selectivity than K-TiO 2 and N/K-TiO 2 . Indeed, the N/K-TiO 2 -Ag-0.5 sample shows the highest CH 4 yield with rate of 113.84 μmol g −1 h −1 and selectivity of CH 4 (93.71%) under light irradiation. The enhancement might be attributed to the synergy of N/K doping and silver loading. In particular, the N/K doping and the Ag cocatalysts introducing triggered improvement of solar energy utilization and charge separation as well as Ag-induced SPR effect and the K + -induced redistribution of photogenerated charge carriers cooperatively promotes photocatalytic CO 2 conversion into CH 4 . It is expected this work would offer a guide for rational design of K/TiO 2 -based photocatalyst for selectively converting CO 2 into fuels.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Wenjiao Chang,Honghuo Wang,Tingting Wu,Shuting Zhang,Yifan Li,Junying Wang,Yongqiang Yang,Lei Wang
Photocatalytic CO 2 reduction reaction is regarded as a potential strategy to convert greenhouse gases into valuable chemicals. However, achieving photocatalysts with high efficiency and target product selectivity under visible light still faces great challenges. Herein, sub-2 nm RuO 2 @TiO 2 (RTO) nanorods with lattice matching interface are rationally designed and prepared via a hydrothermal reaction step-by-step. Due to the strong interaction of the lattice-matched interface with the Ru-O-Ti bond, new energy levels have emerged at the interface, leading to effective visible light absorbance. Moreover, the photo-generated electrons could be transferred to the RuO 2 efficiently via the lattice-matched interface. As a result, the RTO photocatalyst exhibits superior CO 2 -to-CH 4 conversion performance of 15.6 µmol g −1 with a selectivity of 87.9% under visible light irradiation. Density functional theory (DFT) calculation reveals that the energy barrier of CO* to CO is significantly higher than that of *CHO, resulting in the preferential production of CH 4 . This work provides an effective strategy for designing photocatalyst with promoted visible light absorption and improved product selectivity.
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