ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Xiaoqi Zhu,Lin Chen,Qisheng Fang,Jianli Cheng,Yuefeng Su,Paula Ratajczak,Francois Beguin,Bin Wang
Li-CO2 batteries with attractive characteristics of high energy density power supply and carbon dioxide fixation have attracted widespread attention. However, the lack of suitable cathode catalysts and their unsatisfactory electrochemical performance have impeded their development as promising Li-CO2 batteries for energy storage. Constructing heterojunctions by interfacial engineering to improve performance is considered one of the effective strategies. Herein, heterostructured CuCo2S4-Co9S8 nanosheets are fabricated by a facile hydrothermal method and employed as efficient cathode catalysts for Li-CO2 batteries. The construction of heterojunctions by interfacial engineering has proved as an effective strategy to enhance the electrochemical performance of the Li-CO2 batteries. The delocalized electrons between CuCo2S4 and Co9S8 contribute to a low median charge potential (∼3.6 V), small polarization (0.62 V), high energy efficiency of up to 83%, and outstanding cycle life (480 h) of the CuCo2S4-Co9S8 cathodes. Meanwhile, as a proof of concept, flexible fiber-shaped Li-CO2 batteries based on these cathodes are fabricated and demonstrate boosted flexibility adaptability and provide a stable power supply at various bending conditions.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米技术
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Xueyan Chen,Shuo Hu,Xiaoxiao Qin,Min Chen,Jianghao Zhang,Xiaolei Bao,Changbin Zhang
Ag-based catalysts have been extensively investigated in HCHO oxidation on account of the low price of the Ag precursor and their considerable low-temperature activity. It is known that H2 pretreatment has a remarkable promotion effect on Pt- and Pd- catalysts for HCHO oxidation, whereas the effect of H2 reduction on Ag-based catalysts has been rarely reported, probably due to the coexistence of multiple states of Ag species resulting from the high Ag loading. Herein, we prepared a 1% Ag/Al2O3 (Ag/Al-fresh) catalyst with Ag species in a uniform state and then reduced Ag/Al-fresh with H2 at 600 °C to obtain the Ag/Al-600H2 catalyst. We observed that H2 reduction had a significant influence on the performance of Ag/Al2O3 nanocatalysts in HCHO oxidation. In a dry reaction atmosphere, Ag/Al-fresh and Ag/Al-600H2 exhibited comparable HCHO conversion levels, but Ag/Al-600H2 showed much higher CO2 selectivity than Ag/Al-fresh. The presence of water vapor severely suppressed the HCHO conversion of the Ag/Al-fresh catalyst, while Ag/Al-600H2 showed high water resistance, maintaining high HCHO conversion and CO2 selectivity at 35% RH. Characterization results showed that the Ag species on Ag/Al-fresh and Ag/Al-600H2 were single-atom cationic Ag and metallic Ag nanoparticles, respectively. It was revealed that the Ag0 nanoparticles were more conducive than single-atom Ag+ to formate decomposition, as well as O2 and H2O activation, thus accelerating the conversion of HCOO– and CO intermediates to CO2 and contributing to the higher activity and water resistance of the Ag/Al-600H2 catalyst.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Ruiming Fang,Zhongqing Yang,Zukhra C. Kadirova,Ziqiang He,Ziqi Wang,Jingyu Ran,Li Zhang
The visible-light photocatalytic reduction of CO 2 becomes a vital breakthrough to alleviate the greenhouse effect and achieve carbon neutrality. In this paper, ultrathin g-C 3 N 4 nanosheets of 1.74 nm were constructed, and K + was successfully doped between layers. The yields of CO and CH 4 are 1.65 μmol·g −1 ·h −1 and 0.15 μmol·g −1 ·h −1 , which are 4.70 and 7.27 times higher than the original g-C 3 N 4 , respectively. The ultra-thin nano-lamellar structure shortens the carrier transmission distance, and the intercalation of K + not only promotes the electron transport between g-C 3 N 4 layers but also changes the original hybrid mode of the catalytic system, thus shortening the band gap and adjusting the energy band structure. In addition, the CO 2 adsorption center of the K + intercalated g-C 3 N 4 is transferred from the coordinated carbon atom to the center of the triazine unit, and the binding energy is obviously increased, which strengthens the CO 2 adsorption. Finally, through in-situ DRIFT characterization, it is speculated that the reaction enhancement mechanism is that the modified catalyst promotes the adsorption and activation of CO 2 , resulting in the production of more intermediates, especially more hydrocarbon intermediates, which is more conducive to the photocatalytic reduction of CO 2 .
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Changzhen Wang,Hao Wu,Xiangyu Jie,Xiaoming Zhang,Yongxiang Zhao,Benzhen Yao,Tiancun Xiao
Well-geometric-confined yolk–shell catalysts can act as nanoreactors that are of benefit for the antisintering of metals and resistance to coke formation in high-temperature reactions such as the CO2 reforming of methane. Notwithstanding the credible advances of core/yolk–shell catalysts, the enlarged shell diffusion effects that occur under high space velocity can deactivate the catalysts and hence pose a hurdle for the potential application of these types of catalysts. Here, we demonstrated the importance of the shell thickness and porosity of small-sized Ni@SiO2 nanoreactor catalysts, which can vary the diffusional paths/rates of the diffusants that directly affect the catalytic activity. The nanoreactor with an ∼4.5 nm shell thickness and rich pores performed the best in tolerating the shell diffusion effects, and importantly, no catalytic deactivation was observed. We further proposed a shell diffusion effect scheme by modifying the Weisz–Prater and blocker model and found that the “gas wall/hard blocker” formed on the openings of the shell pores can cause reversible/irreversible interruption of the shell mass transfer and thus temporarily/permanently deactivate the nanoreactor catalysts. This work highlights the shell diffusion effects, apart from the metal sintering and coke formation, as an important factor that are ascribed to the deactivation of a nanoreactor catalyst.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Huan Wang,Shu-Wei Yin,Jianchuan Liu,Weitao Wang,Zhen-Hong He,Kuan Wang,Zhi-Hao Zhao,Zhao-Tie Liu
Ni, especially Ni single atom catalysts (SACs) are the most promising electrocatalyst in the reduction of CO 2 to CO. However, the high energy barrier for the formation of *COOH on Ni SA sites leads to a high overpotential for CO 2 RR, which severely hinders the CO production efficiency. How the coupling effect of Ni SAs and Ni nanoparticles (NPs) sites improve the performance of Ni-based electrocatalysts is interesting to be investigated. Herein, theoretical calculations revealed that the synergy of Ni SAs and Ni NPs could efficiently lower the energy barrier of the *COOH formation via promoting the H 2 O dissociation process to accelerate the *H supply for CO 2 protonation as well as promote the CO 2 adsorption and CO desorption, thus improving catalytic activity. Based on the theoretical study, Ni-N 4 SA coupled with Ni nanoparticles supported on nitrogen-doped carbon nanotubes (Ni-N 4 Ni NP /NCNT) was designed. As electrocatalyst, the Ni-N 4 Ni NP /NCNT showed an ultralow onset overpotential of 60 mV for CO 2 RR-to-CO, and achieves a FE CO of ∼99 % from an overpotential of as low as 160 mV, outperforming state-of-the-art Ni SACs. This work not only sheds new light for the rational synthesis of Ni-based catalysts with both Ni SAs and Ni NPs sites to achieve efficient CO 2 RR to CO, but also offers an in-depth insight for the origin of efficient performance of cooperative Ni SA -Ni NP catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yong Yang,Jianfeng Jiang,Ya-Nan Feng,Zanyong Zhuang,Fei-Fei Chen,Dantong Zhang,Yan Yu
The strong CO 2 adsorption and facile CO desorption are a trade-off issue for CO 2 -to-CO photoreduction pathways. Synchronous optimization of these two steps remains a substantial hurdle and has been less explored. Herein, an O/N mixed coordinated Co-NTA (NTA: nitrilotriacetic acid), featuring an ultralong nanofiber architecture, is reported for efficient CO 2 photoreduction. The mixed coordination can regulate the positions of d -band center of Co sites and also d – p orbital coupling with coordination atoms, which are recognized as main activity descriptors. Consequently, free energies of both steps of CO 2 →*CO 2 and *CO→CO are well optimized, making the CO 2 -to-CO photoreduction pathways more favorable thermodynamically. By contrast, the classic N-coordinated Co-MeIm (MeIm: 2-methylimidazole) and O-coordinated Co-BDC (BDC: 1,4-benzenedicarboxylic acid) suffer from unfavorable CO 2 adsorption and intractable CO desorption, respectively. In addition, achiral NTA molecules can direct the growth of Co-NTA into one-dimensional (1D) nanofibers, while Co-BDC and Co-MeIm possess typical 2D nanosheet and 3D polyhedron architectures. The fast electron transport along the axis directions makes charge-transfer kinetics most efficient over 1D Co-NTA. The thermodynamic and kinetic benefits jointly contribute to the 1.8-fold increase in CO production over 1D Co-NTA.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
·
IF 4.1
Xiangqian Guo,Chenhui Qiu,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction with perovskite can effectively address both energy and environmental issues. Nevertheless, it remains challenging to prepare photocatalysts with suitable hollow tubular structures in rational. Herein, the La 1-x Sr x Co 1-δ Fe δ O 3 nanofiber with a hollow tubular structure was fabricated through an electrospinning method. The hollow nanofiber structure was constructed by doping Sr atoms in the A-site and Fe atoms in the B-site of LaCoO 3 perovskite. The characterization of TEM proved that the hollow tubular structural La 1-x Sr x Co 1-δ Fe δ O 3 nanofiber exhibited an external diameter of about 95 nm and an internal diameter of about 50 nm. The hollow tubular structural La 1-x Sr x Co 1-δ Fe δ O 3 nanofiber showed superior carrier separation ability which could exhibit significant advantages for photocatalytic CO 2 reduction. The CH 3 OH generation rate over the optimized La 0.8 Sr 0.2 Co 0.7 Fe 0.3 O 3 nanofiber could reach 5.25 µmol⋅g −1 ⋅h −1 . This work highlighted an electrospinning strategy to build a hollow tubular structural La 1-x Sr x Co 1-δ Fe δ O 3 nanofiber for enhancing photoreduction CO 2 .
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Mian Zhu,Chao Lyu,Feng Dai,Jingxian Liu
To develop an environmentally friendly CO 2 capture technology, composite adsorbent beads were synthesized through the in situ growth of ZIF-8 in a nanocellulose gel scaffold prepared from pine needles-derived cellulose. The composite beads were subsequently functionalized with three ionic liquids ([BMIM][PF 6 ], [BMIM][BF 4 ], and [EMIM][TF 2 N]), which induced partial dissolution of the nanocellulose. This process resulted in the formation of unique wrinkled microstructures, resembling rice grains in morphology but exhibiting higher compressive strength. Notably, the IL-loaded CNF/ILs@ZIF-8 composites exhibited significantly superior adsorption performance over unmodified CNF@ZIF-8 (CZ) beads. Under static conditions (3 bar, 273 K), all three functionalized CNF/ILs@ZIF-8 variants enhanced CO 2 uptake capacities by > 46 %, with the [BMIM][PF 6 ] modified beads retaining 85.36 % of initial adsorption capacity after six adsorption–desorption cycles. Furthermore, under competitive dynamic adsorption (1 bar, 273 K), the [BMIM][BF 4 ] modified beads achieved a 43.12 % enhancement in CO 2 /N 2 selectivity compared to CZ. This work provides a MOF granulation strategy with process safety and environmental sustainability, potentially extending MOF applications in gas adsorption technologies.
研究领域:
环境科学
·
材料工程
·
化学工程
·
纳米技术
·
气体吸附
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Peng Wei,Kaidi Guo,Yahong Xie,Xueli Huang
CO2 foams are of great importance in oil recovery but challenging in some aspects like long-term stabilization and time-separated conflict. In this work, a stability-enhanced switchable foam was fabricated using bis-(2-hydroxyethoxy) olefine amine (BOA) and trace amounts (0.05 wt %) of cationic-modified cellulose nanofibers (CCNFs). The CCNF was developed using sequentially functionalized CNF with diamine groups, which were essential to promote the aqueous dispersibility and a key for strengthening the stabilization of foam. The combination of similarly charged CCNFs and BOA in the presence of CO2 contributed to both surface activity and viscoelasticity. It was demonstrated that CCNFs were entangled and stacked to form the compact films and possessed the ability to costabilize the lamellae, as observed by microscopic studies. In addition, the intermolecular H-bonds were promoted in the binary system after being protonated by CO2 and thus balancing the electrostatic forces, as explored by spectroscopy characterizations. The soft fibrous structure of the CCNF was also capable of wrapping gas bubbles in the form of a functional membrane with both low gas permeability and high surface potential, which slowed down the coarsening and coalescence. Of particular interest is that the reversible protonation state of CCNF-BOA complexes upon the alternate treatment with CO2/N2 led to reversible fast foaming/defoaming, which would be beneficial to construct the steerable plugging in the sand pack. This work is expected to provide a new direction and application of the CO2 responsive foam stabilized by similarly charged nanocellulose fibers in oilfield development.
研究领域:
石油工程
·
材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 8
·3604-3623
·
IF 3.5
Wang Xintong,Yang Jiang,Chen Xu,Wang Yefei,Yang Zhen,Ding Wei
To mitigate CO 2 corrosion in the oil and gas industry, a green non-toxic β -N-butyl amino propionic acid (BAA) was synthesized using a low-energy and zero-waste one-pot method. The effectiveness of BAA as a corrosion inhibitor for N80 steel in CO 2 -saturated brine water was investigated through experimental measurements and theoretical modeling. The results demonstrate that BAA functions as an effective mixed-type corrosion inhibitor. BAA molecules interact with F (1 1 0) with the–COO– and–NH 2 + -moiety in the hydrophilic head group, and the hydrophobic groups are adsorbed on the steel surface in a configuration 45° away from the steel surface. The adsorption is a mixture of physical and chemical processes and is consistent with the Langmuir isothermal adsorption formula. When the concentration is greater than 50 ppm, a complete corrosion inhibitor film with high hydrophobicity can be adsorbed on the steel surface, which can effectively impede the diffusion of corrosive species from brine to the steel surface. Graphical abstract
研究领域:
腐蚀科学
·
材料工程
·
环境化学
·
石油天然气工业
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Kai Ma,Yao Luo,Jietao Wang,Xu Chang,Tong Liu,Yao Wang,Mingyue Ding
Developing robust fuel electrodes with high catalytic activity and stability under CO/CO 2 atmospheres is critical for reversible solid oxide fuel cells (RSOFCs). Here, we report a novel A-site-deficient perovskite Sr 1.95 Fe 1.5 Mo 0.3 Ni 0.2 F 0.1 O 6-δ (SFMNF) synthesized via electrospinning, combining Ni 2+ (B-site cation) and F - (anion) co-doping to enhance CO 2 electrolysis and syngas oxidation performance. Physicochemical characterization reveals that F-doping lowers the crystallization temperature, increases oxygen vacancy concentration, and strengthens CO 2 chemisorption. Reduction under H 2 induces exsolution of Ni 3 Fe alloy nanoparticles. The SFMNF electrode achieves a current density of 233 mA cm -2 at 1.3 V and 750°C in CO:CO 2 =2:1 atmosphere, with 36.2% higher activity than the pre-reduced state. Electrochemical impedance and distribution of relaxation time analyses identify CO 2 adsorption/dissociation as the rate-limiting step. The cell demonstrates exceptional durability over 50 redox cycles and 85-hour of operation without carbon deposition. This work highlights dual doping as an effective strategy to tailor perovskite properties for efficient CO 2 utilization in RSOFCs.
研究领域:
能源材料
·
电化学
·
催化
·
纳米技术
·
固体氧化物燃料电池
·
CO2利用
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Li Yin,Meiling Li,Hailun Xia,Shanshan Mao,Fangyuan Gai,Hao Wang
The gas separation performance of hybrid carbon molecular sieve membranes is critically influenced by the particle size of the fillers. Herein, ZIF-8 crystals of different sizes (≈50 nm, ≈500 nm, and ≈1 µm) are used as fillers to synthesize a series of ZIF-8-derived-carbon hybrid carbon molecular sieve membranes with high filler loading. As the ZIF-8 crystal size increases from nanoscale to microscale, the CO 2 permeability of the resulting hybrid carbon molecular sieve membrane for a CO 2 /CH 4 binary mixture increases, reaching 9965 Barrer with a selectivity of 28.05. This trend highlights a clear correlation between filler size and gas separation performance of the hybrid carbon molecular sieve membranes. Microscale ZIF-8-derived-carbon offers synergistic advantages by providing abundant hierarchical pores for molecular sieving and continuous, long pathways for efficient gas transport, while preventing particle aggregation under high loading. Our finding provides valuable insights for the further development of high-performance hybrid carbon molecular sieve membranes.
研究领域:
材料科学
·
膜分离技术
·
化学工程
·
气体分离
·
纳米材料
·
多孔材料
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）