Materials
·
2025
·Vol. 18
·期 17
·4148
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IF 3.2
Xiang Liu,Fujiang Huang,Xiang Shi,Hangmin Xu,Jian Xu,Xingwang Zhu
Alongside the gradual progress of industrialization and the continuous development of human society, the problems of environmental pollution and energy crisis have become increasingly prominent. Semiconductor photocatalysis is a promising solution to these challenges. The photocatalytic reduction of CO2by TiO2to produce carbon monoxide and methane is a process which has been identified as a means of developing clean energy. In this paper, two-dimensional TiO2(2D-TiO2) was synthesized via a one-step solvothermal method, and one-dimensional TiO2(1D-TiO2) was obtained through a hydrothermal process. Their photocatalytic CO2reduction performances were systematically investigated. The results show that 2D-TiO2exhibits superior catalytic activity compared to 1D-TiO2, which can be attributed to its lamellar structure, larger specific surface area, and improved hydrophilicity, providing more active sites and faster reaction kinetics. To further reveal the reaction mechanism, density functional theory (DFT) calculations were carried out using VASP with the GGA–PBE functional, PAW potentials, and a plane-wave cutoff energy of 520 eV. A 3 × 3 × 1 Monkhorst–Pack grid was used for Brillouin zone integration, and all possible adsorption configurations of CO2*, COOH*, and CO* intermediates on the 2D-TiO2surface were evaluated. The results confirm that 2D-TiO2stabilizes key intermediates more effectively, thereby lowering the energy barrier and facilitating CO2reduction. These findings demonstrate that structural modulation of TiO2significantly influences its photocatalytic performance and highlight the great potential of 2D-TiO2for efficient CO2conversion and clean energy applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Yujie Tan,Ran Sun,Hui Xu,Yuan Yuan,Xingang Liu,Andrew E.H. Wheatley,Renxi Zhang
By employing a non-metal doping strategy, we systematically achieved the stabilization and synergistic modulation of both surface defects and spin polarization within the wide-bandgap semiconductor. This platform is crucial for advancing key applications in both environmental remediation and energy conversion. Optimized photocatalytic activity in TiO 2 is achieved by tailoring its electronic structure through a template-assisted route, where boron acids act simultaneously as dopants and mesopore-directing agents. Mechanistically, advanced techniques including PAS, EXAFS, OCPD and DFT calculations reveal spin polarization in TiO 2 arises when interstitial boron pairs with nearby oxygen vacancies to form B–Ov complexes that stabilize vacancy-derived defect states and, via local dipoles and distortion of TiO 6 octahedron, break spin degeneracy near Fermi level (E f ), thereby suppressing spin-allowed recombination and enhancing photocatalytic charge utilization. Notably, employing boron also enables precise control of hierarchical porosity and surface area in metal oxides. The resulting TiO 2-x bearing spin-polarized B–Ov complexes delivers CO from CO 2 at 24 µmol h⁻¹ g⁻¹ with high selectivity and degrades tetracycline under visible light within 2 h (k = 0.016 min⁻¹), which are 6- and 16-fold faster than pristine TiO 2 and TiO 2 -based photocatalysts reported under similar TC degradation conditions. This work presents a significant advance in the methodology for constructing next-generation free-standing photocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xia Bai,Jingmin Ge,Huanhuan Yang,Huiwen Tian,Xueqi Liu,Shiying Li,Zhikun Peng,Yaxi Li,Jiahao Wang,Hongpo Liu,Qun Xu
Building of grain boundary (GB) in Cu-based catalysts has been demonstrated to be an efficient strategy to control the product selectivity of electrochemical CO 2 reduction reaction (eCO 2 RR). However, the fabrication and modulation of GBs in Cu are still challenging. In this study, a series of bare Cu catalysts with controllable density of Cu(111) GBs were investigated systematically for eCO 2 RR. These catalysts exhibit superior eCO 2 RR performance for syngas production with a high FE of ∼80 % and tunable H 2 /CO ratio of 0.46–2.78. Three-dimensional wormlike Cu with abundant (111) GBs displays a stable H 2 /CO ratio of ∼0.5 over a wide potential range from −0.9 to −1.2 V ( vs. RHE). In situ Raman and ATR-SEIRAS spectroscopy combined with DFT calculations reveal that Cu(111) GBs enhance the adsorption of CO 2 , lower the energy barriers of CO 2 to *COOH and *CO, further highlighting the potential to control syngas production with desirable proportion over Cu-based catalysts.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Mengyang Xu,Bingqing Chang,Jinze Li,Huiqin Wang,Pengwei Huo
The assembly of different Metal organic framework (MOFs) into hybrid heterostructures has proven to be a promising strategy that can effectively break through the limited regulatory capacity of single metal sites. Here, an S-scheme heterostructure (Fe 3 Ni-MOF) based on homologous ligands (1,4-phthalic acid) of ultra-thin Ni-MOF and Fe-MOF nanoparticles with directional electron transport channels, was developed and used it for photoreduction of CO 2 . Under the S-scheme electric field mechanism, the photogenerated carrier can achieve efficient directional separation through Fe–O–Ni atomic bond, which significantly reduces the energy barrier of the rate-determining step. Results show that the performance of Fe 3 Ni-MOF (63.5 μmol g –1 ) was 20 and 3.2 times higher than that of Ni-MOF and Fe-MOF, respectively, and exhibits excellent CO selectivity (96.4%) and stability. Transmission electron microscopy and atomic force microscopy revealed the two-molecular-layers structure of Ni-MOF and the micro-assembly structure of Fe 3 Ni-MOF, which can shorten the electron transport distance and increase the molecular mass transfer rate. X-ray photoelectron spectroscopy, electron spin resonance and electron density difference calculations reveal that interfacial electric fields and atomic bonds work together to promote directional carrier separation, resulting in the accumulation of holes on Ni-MOF and electrons on Fe-MOF. The Gibbs free energy calculation and in-situ Fourier transformed infrared spectroscopy validate that the micro-assembled S-scheme heterostructures with directional electron transport channels can significantly reduce the activation energy barrier of the reaction. This study not only proves the feasibility of constructing MOFs S-scheme heterostructures using homologous ligands, but also provides a new way to overcome the limitations of monometallic MOFs. This strategy is expected to open up a new avenue to design efficient photocatalysts.
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Advanced Science
·
2022
·Vol. 9
·期 16
·2105292
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IF 17.521
Yawen Jiang,Xinyu Wang,Delong Duan,Chaohua He,Jun Ma,Wenqing Zhang,Hengjie Liu,Ran Long,Zibiao Li,Tingting Kong,Xian Jun Loh,Li Song,Enyi Ye,Yujie Xiong
Structural reconstruction is a process commonly observed for Cu-based catalysts in electrochemical CO 2 reduction. The Cu-based precatalysts with structural complexity often undergo sophisticated structural reconstruction processes, which may offer opportunities for enhancing the electrosynthesis of multicarbon products (C 2+ products) but remain largely uncertain due to various new structural features possibly arising during the processes. In this work, the Cu 2 O superparticles with an assembly structure are demonstrated to undergo complicated structure evolution under electrochemical reduction condition, enabling highly selective CO 2 -to-C 2+ products conversion in electrocatalysis. As revealed by electron microscopic characterization together with in situ X-ray absorption spectroscopy and Raman spectroscopy, the building blocks inside the superparticle fuse to generate numerous grain boundaries while those in the outer shell detach to form nanogap structures that can efficiently confine OH − to induce high local pH. Such a combination of unique structural features with local reaction environment offers two important factors for facilitating C−C coupling. Consequently, the Cu 2 O superparticle-derived catalyst achieves high faradaic efficiencies of 53.2% for C 2 H 4 and 74.2% for C 2+ products, surpassing the performance of geometrically simpler Cu 2 O cube-derived catalyst and most reported Cu electrocatalysts under comparable conditions. This work provides insights for rationally designing highly selective CO 2 reduction electrocatalysts by controlling structural reconstruction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Liwei Sun,Lipeng Wang,Meilin Yin,Shaokun Tang
Direct utilization of low-concentration CO 2 is of importance to mitigate the global warming and reduce energy consumption. Herein, a new bi-functional ionic liquid-grafted material was fabricated for CO 2 /N 2 selectivity and diluted CO 2 cycloaddition reaction. Following the preparation of 1-carboxymethyl-3-methoxy ethyl-imidazolium chloride ([CmMOEim]Cl) containing carboxyl and ether group, MIL-53(Al) was used for directly chemical grafting of the ionic liquid to obtain [CmMOEim]Cl@MIL-53(Al). CO 2 capture capacity of [CmMOEim]Cl@MIL-53(Al) reached up to 70 cm 3 CO 2 /g sorbent at 25 °C and 0.1 MPa, which was higher than that of two individual components. Cyclopropyl carbonate of 97 % yield was obtained at 110 °C, 3 MPa of initial 50 vol% CO 2 /N 2 pressure and 4 h with 2.4 wt% [CmMOEim]Cl@MIL-53(Al)-0.4 under solventless and co-catalyst-free condition. Various terminal cyclocarbonates were synthesized with above 90 % yield. In addition, the heterogeneous catalyst was separated from reaction system by simple centrifugation and the yield of cyclopropyl carbonate was higher than 90 % after 12 cycles owing to the chemical grafting of [CmMOEim]Cl on MIL-53(Al).
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Yang Haozhou,Guo Na,Xi Shibo,Wu Yao,Yao Bingqing,He Qian,Zhang Chun,Wang Lei
Cobalt phthalocyanine immobilized on carbon nanotube has demonstrated appreciable selectivity and activity for methanol synthesis in electrocatalytic CO 2 /CO reduction. However, discrepancies in methanol production selectivity and activity between CO 2 and CO reduction have been observed, leading to inconclusive mechanisms for methanol production in this system. Here, we discover that the interaction between cobalt phthalocyanine molecules and defects on carbon nanotube substrate plays a key role in methanol production during CO 2 /CO electroreduction. Through detailed operando X-ray absorption and infrared spectroscopies, we find that upon application of cathodic potential, this interaction induces the transformation of the planar CoN 4 center in cobalt phthalocyanine to an out-of-plane distorted configuration. Consequently, this potential induced structural change promotes the transformation of linearly bonded *CO at the CoN 4 center to bridge *CO, thereby facilitating methanol production. Overall, these comprehensive mechanistic investigations and the outstanding performance (methanol partial current density over 150 mA cm −2 ) provide valuable insights in guiding the activity and selectivity of immobilized cobalt phthalocyanine for methanol production in CO 2 /CO reduction.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Hanwen Wang,Jiawei Wang,Hangyuan Zhang,Xinyang Wang,Xiaoping Rao
Emulsion-based delivery systems are extensively employed for encapsulating functional active ingredients, protecting them from degradation, and enhancing bioavailability and release efficiency. Here, a CO 2 -responsive surfactant synthesized from rosin displays rapid responsiveness to CO 2 at room temperature, transitioning reversibly switches between active and inactive states multiple times. The dual tertiary amines on the rosin rigid structure contributes to its CO 2 sensitivity. When in its active cationic form, in conjunction with silica nanoparticles , it exhibits desired Pickering emulsification performance across various oil phases. In the Pickering emulsion loaded with quercetin , the encapsulation efficiency and loading efficiency reached 80.50% and 0.69%, respectively, with stability lasting at least 30 days. The system provides robust protection for quercetin against external factors, such as UV and heat, revealing sustained release effects. This study investigated the potential of using rosin-based CO 2 -responsive surfactants alongside nanoparticles to design stable Pickering emulsion systems for active substance encapsulation and sustained release.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Lingyu Shao,Feng Xu,Zhicheng Wu,Chang Liu,Chengjin Pan,Yifan Wang,Zhengda Yang,Tao Wang,Longchao Yao,Chenghang Zheng,Xiang Gao
Advancement of the absorbent for CO 2 capture is essential in optimizing the performance and reducing the negative environmental effects associated with this technology. Despite ammonia's promise as an absorbent, the volatility limits its practical application and creates potential environmental pollution . Therein, we assess various additives (amino acids, carbonates, and alkanolamines) for ammonia-based solvents using multi-stage circulation absorber from the viewpoints of aerosol emission, ammonia emission, and CO 2 capture efficiency. Experimental findings reveal that ammonia volatilization can be inhibited by the protonation of free ammonia by carboxyl groups and the formation of hydrogen bonding between amino/hydroxyl groups and ammonia, with ammonia emission reduced by 21.7 %, aerosol emission reduced by 26.5 %, and CO 2 capture efficiency increased to a maximum of 87.8 % under the condition of adding histidine . Moreover, the experiment highlights a positive correlation between total ammonia emission and aerosol concentration/diameter. Additionally, tests combining source abatement with water wash exhibit up to 50.5 % aerosol removal efficiency and up to 76.6 % ammonia removal efficiency. To further mitigate emissions, a comprehensive approach is proposed, achieving an 84.4 % reduction in ammonia emission and a 61.9 % reduction in aerosol emission. Finally, a method for recycling ammonia for desulfurization is suggested.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Luotian Lv,Yao Liu,Yankai Huang,Tong Li,Han Feng,Yongqing Wang
Since the intensification of global environmental pollution and energy shortages, photocatalytic CO 2 reduction reaction (CO 2 RR) has emerged as a promising strategy to convert solar energy into clean chemical energy. Herein, we construct a robust and efficient heterojunction construction photocatalyst for CO 2 RR, composed of the highly reactive CeNi quantum dots (CeNi QDs) and nickel metal–organic layer (Ni-MOL) ultrathin nanosheets. This design facilitates the rapid separation of photogenerated charge carriers, as confirmed by X-ray photoelectron spectroscopy (XPS), photoluminescence spectroscopy (PL) and other characterizations. Mechanistic studies with in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and the d-band center calculation indicate that the propensity of photocatalyst for CO 2 absorption and CO desorption, leading to high performance and selectivity. The optimized loading amount of CeNi quantum dots and modified structure result in a CO yield of 30.53 mmol·g −1 within 6 h under irradiation. This work not only paves a new and convenient way for developing high-activity quantum dot materials for CO 2 RR but also exploits novel avenues to fabricate more heterojunction composites for solar energy conversion.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Yanan Jiang,Huayu Sun,Yuzhen Fang,Cuijuan Zhang,Yuan Liu
The sintering issue of Ni nanoparticles seriously limits the practical application of the Ni-based catalysts for CO 2 methanation. This work demonstrates that the La- and Ce- dual-promoted Ni/ZrO 2 shows better durability at 600 ºC and 60000 mL g cat −1 h −1 over 200 h compared with the La- or Ce- single-promoted. The composition and microstructure characterization indicates that the dispersion and sintering resistance of Ni nanoparticles is enhanced with the dual-promoted catalysts. Both depth profile of X-ray photoelectron spectroscopy and density functional theory calculation show that in the La- and Ce- dual-promoted Ni/ZrO 2 , the reduced dissolution of Ce into ZrO 2 lattice and the spread of La on ZrO 2 surface by forming a La 2 O 3 -CeO 2 solid solution improves the dispersion and stability of Ni nanoparticles. This work provides a facile strategy to mitigate the sintering of Ni nanoparticles and thus improve the stability of Ni-based catalysts for CO 2 methanation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhilv Chen,Tao Wang,Chao Li,Mengxiang Fang,Wei Chen,Ximing Hu,Wei Zhang,li Zhang,Wenyang Fan,Shaojuan Zeng
In recent years, a large number of studies have shown that amine based water-lean absorbents formed by amines and organic solvents exhibit high capture efficiency and low regeneration energy consumption in CO 2 capture. However, there is a lack of research that combines molecular level structure with macroscopic properties. In order to optimize the performance of amine based homogeneous water-lean absorbents by utilizing the properties of organic solvents, and to explore the correlation between the macroscopic properties of the absorbents (CO 2 capacity, removal efficiency, regeneration rate, regeneration efficiency, etc.) and the molecular structure of the absorbent components. We used experiments and molecular dynamics to study the linear terminal diamine DMEDA and non-proton polar solvent (DMF, DMPA, NMP, SFL, DMSO) system. It was found that the absorption and desorption performance of water-lean solvents was higher than that of aqueous solutions 30 wt% MEA and 30 wt% DMEDA, among which EFH with DMF as the solvent has better comprehensive performance. The molecular dynamics simulation was built to describe the solution structures of these absorbents. Through RDF calculations, the unique behavior of DMEDA in non-proton polar solvent was revealed on molecular level, it was found that organic solvents tend to aggregate with DMEDA molecules to form large molecular clusters, while CO 2 molecules may diffuse through ordered pore structures, resulting in a significant improvement in the capture performance. And it was found that there is a quantitative relationship between the intensity of intermolecular interaction between DMEDA and CO 2 and the removal efficiency change in DMEDA water-lean absorbents. A functional relationship was fitted, and a preliminary and rapid method for determining capture performance through molecular dynamics was proposed.
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