ACS Applied Engineering Materials
·
2023
·
IF 0
Sheng Chang,Yimin Xuan,Qi Wang,Kui Wang
Bimetallic catalysts are ideal candidates for boosting electrochemical CO2 reduction reaction (CO2RR). However, these catalysts have largely relied on tedious synthesis technology and play electrolytic role with the help of a metal substrate or gas diffusion electrode. Herein, noble metal-free In–Sn nanoparticles (NPs) with a core–shell structure that contains a hybrid In–Sn core and native Sn-doped In2O3 shell have been successfully grown on the copper foam by the potential-driven volume diffusion strategy. These NPs which spontaneously result in the formation of the In–Sn bimetallic interface by adjusting the element composition significantly boost the yield of CO2 reduction into formate over a wide potential window (−0.77 to −1.17 V versus reversible hydrogen electrodes) compared with pure single-metal counterparts. The optimized In–Sn NPs deliver a great partial current density of 57.6 mA cm–2 and high faradaic efficiency of 97.0%, a remarkable performance in comparison to the state-of-the-art reported bimetallic catalyst. Such excellent performance is revealed via in situ Raman analyses and theoretical calculations, indicating that the unique structure of In–Sn NPs with the In–Sn bimetallic interface favorably regulates the reaction dynamics and facilitates the adsorption of the *OCHO intermediate.
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DOI
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 40
·405201
·
IF 3.5
Zhuohua Chen,Xiaoli Jin,Qing Lan,Xin Li,Qunzeng Huang,Wenmin Liu,Yuwei Guo,Haiquan Xie,Liqun Ye
Photocatalytic CO2 reduction is considered to be an appealing way of alleviating environmental pollution and energy shortages simultaneously under mild condition. However, the activity is greatly limited by the poor separation of the photogenerated carriers. Ion doping is a feasible strategy to facilitate the charge transfer. In this work, Ni-doped Bi4O5I2 photocatalyst is successfully fabricated using a one-pot hydrothermal method. A few doping levels appear in the energy band of Bi4O5I2 after Ni doping, which are used as springboards for electrons transition, thus promoting photoexcited electrons and holes separation. As a consequence, a remarkably enhanced yield of CO and CH4 (6.2 and 1.9 μmol g−1 h−1) is obtained over the optimized Bi4O5I2-Ni15, which is approximately 2.1 and 3.8 times superior to pure Bi4O5I2, respectively. This work may serve as a model for the subsequent research of Bi-based photocatalysts to implement high-performance CO2 photoreduction.
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高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Luming Qi,Yu Han,Gaozhi Bai,Qing Liu,Zhaoyang Fei,Xian Chen,Zhuxiu Zhang,Jihai Tang,Mifen Cui,Xu Qiao
Amine adsorbents have been widely investigated for direct CO 2 capture from air. However, the low amine efficiency of the widely-studied amine sorbents is the critical factor to hinder the practical application under dry conditions. Herein, we developed the brush-like cetyltrimethylammonium chloride (CTAC) templating strategy to prepare micro-mesoporous silica nanoparticles (MMSN-X) and TEPA-functionalized adsorbents (MMSN-X/TEPA-Y). The character of samples was investigated by transmission electron microscopy , N 2 adsorption-desorption, Fourier transform infrared spectroscopy, thermal gravimetric analyzer and X-ray photoelectron spectroscopy. The adsorbent (MMSN-30/TEPA-50) with appropriate amount of brush-like CTAC exhibited higher CO 2 adsorption capacities (3.68 mmol/g adsorbent under simulated dry air conditions) than that of the adsorbents with none or less additives. The kinetic and thermodynamic model were applied to investigate the adsorption rate control factors and adsorption behavior of CO 2 adsorbents with brush-like CTAC. Moreover, with the effect of brush-like CTAC, the significant variation of adsorption product (conversion from carbamate (CO 2 /N = 0.5) to carbamic acid (CO 2 /N = 1)) was detected by in situ Fourier transform infrared spectroscopy . These results demonstrated that the combination of CO 2 and amine was altered in the presence of brush-like CTAC and thereby the amine efficiency was enhanced, which could be expected to be an efficient adsorbent for CO 2 from air in practical applications.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Liji Zhang,Yuhang Zheng,Yafei Guo,Shengbin Bai,Meishan Song,Pu Huang,Xinzheng Wei,Jian Sun,Changhai Li,Jiaqing Zhang,Chuanwen Zhao
Thermochemical energy storage (TCES) by means of reversible chemical reactions represents a promising strategy for harnessing renewable energy and recovering industrial waste heat. In this work, alkali metal nitrate promoted MgO composites were synthesized, and the MgO–CO2 working pair was suggested as an alternative candidate for harvesting intermediate-temperature industrial waste heat. However, it remains unclear how operating parameters would affect the heat storage density, and the long-term cycling stability of the alkali metal nitrate promoted MgO composites under harsh conditions close to practical application scenarios needs to be clarified. The objectives of this work are to expound the effects of operating parameters on TCES performance and to evaluate the long-term cycling stability of the alkali metal nitrate promoted MgO composites. With increasing NaNO3 content, the heat storage density of NaNO3–MgO increases dramatically first and then exhibits no significant change. With rising carbonation temperature, the heat storage density of the 10NaNO3–MgO composite increases first and then declines marginally, while it increases with the increasing CO2 partial pressure. Doping alkali metal nitrate eutectic mixtures adversely affects the heat storage density. 10NaNO3–MgO exhibits a high heat storage density of 2291 kJ/kg at 340 °C in 100% CO2. The 10NaNO3–MgO and 10(K–Na)NO3–MgO composites suffer a significant decline in heat storage density within 10 consecutive cycles, while 10(Li–Na)NO3–MgO retains good stability with a slight decrease of heat storage density from 1073 to 770 kJ/kg in 50% CO2. The desired 10(Li–Na)NO3–MgO is suggested as a promising material for TCES application.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ke Wang,Chuanjiang Yang,Pengfei Zhao,Edward J. Anthony
The addition of molten Na 2 CO 3 can drastically accelerated the extremely slow sorption kinetics of Li 4 SiO 4 -based CO 2 sorbents in the sorption enhanced reforming process. However, the lack of a unified consensus about the effect of doped Na 2 CO 3 on the CO 2 capture process, now delays the development of more-effective Li 4 SiO 4 sorbents. Here, sorption tests, sturactural characterzations and periodic density functional theory calculations were combined to develop a better mechanistic understanding CO 2 sorption on Na-doped Li 4 SiO 4 . The Na-doped Li 4 SiO 4 exhibited a better CO 2 capture performance than pure Li 4 SiO 4 even below the melting point of any eutectic mixtures. Structural characterizations revealed that rather than generating physical favorable characteristics, the Na doping substituted at the Li site and created lithium–sodium orthosilicates (Li 4-x Na x SiO 4 ). Theoretical calculations agreeing with experimental results further demonstrated that Li 4-x Na x SiO 4 presented a weaker Na-O bond and generated more active phases (quasi Li 2 O groups) for larger sorption energies, more charge transfers and stronger CO 3 2– bond formation, in turn providing more reactive sites for enhanced CO 2 chemisorption as comparing with pure Li 4 SiO 4 . Finally, we propose a new and unified sorption mechanism independent of the traditional “melting layer” explanation.
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高影响因子
Advanced Energy and Sustainability Research
·
2022
·Vol. 3
·期 6
·2100200
·
IF 0
Ping She,Yuanyuan Qi,Tengfei Bao,Hongbang Rui,Buyuan Guan,Heng Rao,Jun-Sheng Qin
Molecular catalysis for photocatalytic CO 2 reduction (PCR) has recently attracted much attention, whereas its scaled practical application is usually limited by the difficulty of recycling and its photochemical instability in homogeneous solutions. Immobilization of molecular catalysts on solid matrices, that is, covalent bonds or noncovalent interactions, provides a great blueprint to tackle this issue. Herein, a bioinspired self-supporting phthalocyanine@ZnIn 2 S 4 (Pc@ZnIn 2 S 4 ) foam by growing ZnIn 2 S 4 nanosheets on the commercialized polyurethane foam (PF) followed by loading amino-modified cobalt phthalocyanine (CoPc–NH 2 ) is developed. The self-supporting Pc@ZnIn 2 S 4 PF carrier can be directly taken out of the reaction system for the next reaction cycle without any other procedures. The optimized Pc@ZnIn 2 S 4 PF demonstrates superior PCR efficiency under visible light ( λ = 420 nm), achieving 474.65 μmol CO g −1 catalyst after 8 h. The superior PCR performance is attributed to the elevated light-harvesting ability induced by the porous foam structure and the enhanced charge separation efficiency facilitated by the dimension-matched interface between ZnIn 2 S 4 and Pc. The special design of the immobilization molecular catalyst on solid supporters presented herein develops an efficient strategy for solar-driven energy conversion.
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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.
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高影响因子
FUEL
·
2024
·
IF 6.7
Jiaxi Yang,Dan Gao,Heng Zhang,Qun Yi
The efficient capture of carbon dioxide (CO 2 ) by porous ionic liquids (PILs) has become one of the important ways to deal with the greenhouse effect and enhance environmental protection. In order to enhance the CO 2 capture efficiency of PILs, 2 amino-functional ionic liquids (ILs) were synthesized in deionized water: tetraethylenepentamine-2-methylimidazole ([TEPA][MIm]) and diethylenetriamine-2-methylimidazole ([DETA][MIm]). 2 zeolite imidazolidin-8 frames (ZIF-8-W and ZIF-8-M) were prepared in methanol and deionized water. The performance of the material was verified through FT-IR infrared spectroscopy, TGA-DTG curves, XRD spectra, adsorption desorption curves, and corrosive changes. Based on this, the porous ionic liquid ZIF-8-W/[TEPA][MIm] with the best performance and ZIF-8-W with the best environmental friendliness were successfully constructed. The chemical reaction mechanism of CO 2 in PILs were explored. The results showed that the thermogravimetric temperature of all materials was greater than 370 K, and the difference in adsorption capacity between ZIF-8-W and ZIF-8-M was only about 36.3 ml/g, the maximum mass change rates of the two ILs after immersion in ceramic and stainless steel tubes for 7 days were only 0.78 % and 0.29 %, respectively. On the premise of ensuring fluidity, the maximum capture capacity of ZIF-8-W/[TEPA][MIm] for pure CO 2 reached 2.22 mol/mol PILs, and the maximum capture capacity for CO 2 in artificial flue gas reached 2.03 mol/mol PILs, which was 21.9 % and 31.6 % higher than the maximum capture capacity of pure ionic liquids, respectively. When [TEPA][MIm] in PILs reacts with CO 2 , it conforms to the characteristics of “zwitterions”.
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高影响因子
Advanced Powder Materials
·
2026
·
IF 26.8
Minghao He,Zhenghui Tian,Rui Zhang,Yang Qu,Guofeng Wang
A B S T R A C T The key for photocatalytic CO 2 reduction in pure water lies in constructing active sites that possess both rapid charge transfer and efficient CO 2 adsorption. Here, atomically dysprosium (Dy)-cobalt (Co) dual sites anchored g-C 3 N 4 (CN) microtube were successfully fabricated by a precoordination-thermopolymerization strategy, in which Co 2+ and Dy 3+ ions are selectively coordinated with melamine and cyanuric acid, respectively, prior to thermal polymerization. The optimized Co 1 Dy 1 /CN catalyst delivers a CO yield of 240.55 μmol·g −1 and a CH 4 yield of 68.70 μmol·g -1 in pure water without sacrificial agents, representing ∼8.0-fold and ∼4.6-fold enhancements over pristine CN, respectively, superior to most reported single-atom photocatalysts. According to femtosecond transient absorption spectroscopy, theoretical calculation, and in situ techniques, the superior catalytic activity originates from the synergistic interaction between Dy and Co dual active sites. Specifically, Dy-possessing abundant unoccupied 4f orbitals-functions as an electron reservoir that facilitates directional electron transfer toward the Co sites, accelerating charge extraction by 8.4-fold and enhancing electron transfer kinetics by 1.5-fold. This electron enrichment at the Co centers induces a downshift in the Co d -band center, which further strengthens CO 2 adsorption and activation at the Co sites with inherent CO 2 affinity. In this paper, resent the lanthanide-empowered strategy to overcome charge dynamics limitations in cobalt single-atom catalysts. Dysprosium serves as an atomic electron reservoir adjacent to cobalt sites in dual sites centers, enabling synergistic CO2 reduction. Multimodal analysis (XAS, in situ spectroscopy, fs-TA, and DFT) reveals Dysprosium to cobalt electron transfer and d-band center optimization mechanisms. Download: Download high-res image (269KB) Download: Download full-size image
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高影响因子
NANOTECHNOLOGY
·
2018
·Vol. 29
·期 15
·154005
·
IF 3.404
Chunyang Dong,Songchang Hu,Mingyang Xing,Jinlong Zhang
A spatially separated, dual co-catalyst photocatalytic system was constructed by the stepwise introduction of RuO2 and Au nanoparticles (NPs) at the internal and external surfaces of a three dimensional, hierarchically ordered TiO2−SiO2 (HTSO) framework (the final photocatalyst was denoted as Au/HRTSO). Characterization by HR-TEM, EDS-mapping, XRD and XPS confirmed the existence and spatially separated locations of Au and RuO2. In CO2 photocatalytic reduction (CO2PR), Au/HRTSO (0.8%) shows the optimal performance in both the activity and selectivity towards CH4; the CH4 yield is almost twice that of the singular Au/HTSO or HRTSO (0.8%, weight percentage of RuO2) counterparts. Generally, Au NPs at the external surface act as electron trapping agents and RuO2 NPs at the inner surface act as hole collectors. This advanced spatial configuration could promote charge separation and transfer efficiency, leading to enhanced CO2PR performance in both the yield and selectivity toward CH4 under simulated solar light irradiation.
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高影响因子
Applied Materials Today
·
2022
·
IF 8.663
Weibin Zhang,Touwen Fan,Zhen Yang,Ruipeng Yu,Xinjuan Zeng,Yonghang Xu,Min Zhang,Huawen Hu,Jian Zhen Ou,Lirong Zheng
While the relatively complex chemical composition of Prussian blue analogues (PBAs) allows a high degree of flexibility in tuning the catalytic performances toward CO 2 -based copolymerization , little is known regarding the influence of the crystal phase. Herein, we investigate the impact of the crystal phase tuning of the representative Zn−Co-based PBA on CO 2 −epoxide copolymerization. The utilization of oxygen-containing tert ‑butanol molecules ( t BuOH) replaces water molecules from the Zn active center within the PBA-based nanosheets, inducing the crystal transformation from conventionally cubic to rhombohedral. The rhombohedral phase can be formed as clusters dispersed within the amorphous matrix, exhibiting the most active and selective CO 2 −epoxide copolymerization performance with a turnover number of 31,250 g/g Zn compared to that of long-range ordered cubic and rhombohedral counterparts. Such an improvement is ascribed to the abundant exposed Zn-O active centers enabled by the replacement of t BuOH molecules and rhombohedral coordination. Density functional theory calculation indicates different average adsorption energies for cyclohexene oxide (CHO) and CO 2 (-5.45 vs. -0.02 eV) on the (001) surface, implying the initialization of copolymerization from the adsorption of CHO onto the Zn-O active centers. This work provides a feasible approach to enable on-demand manipulation of catalytic performances of emerging PBAs.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Wenji Zheng,Ziheng Li,Tianqi Sun,Xuehua Ruan,Yan Dai,Xiangcun Li,Chuling Zhang,Gaohong He
Metal organic frameworks (MOFs) based mixed matrix membrane (MMM) for CO 2 capture shows insufficient CO 2 permeability due to random disperse of MOFs in form of individual particle. Therefore, in this work, a continuous MOFs transport pathway for CO 2 with low resistance was constructed in the MMM by assistance of electrospun nanofiber . Specifically, PAN electrospun nanofiber mat (NFM) was utilized as skeleton to obtain continuous ZIF-8 nanofibers. Then flexible polyethylene glycol (PEG) molecules were photo-polymerized in situ into the inner-voids within ZIF-8@PAN NFM to form dense membrane . As a result, ZIF-8 particles are distributed in PEO matrix continuously, leading to a low-resistance transport pathway for gas molecules in MMM, which is proved by the cross-sectional SEM images. Furthermore, the higher Tg of ZIF-8@PAN-x/PEO MMM by DSC also indicates the good interfacial compatibility between ZIF-8 and PEO. Compared with pure PEO membrane, all the ZIF-8@PAN-x/PEO MMMs present both enhanced CO 2 permeability and CO 2 /N 2 selectivity. The enhanced CO 2 permeability is attributed to the continuous ZIF-8 transport pathway, and the improved selectivity is ascribed to the size screening from nanofibers overlapping and stacking and the tortuous transport pathway. Importantly, compared with ZIF-8/PEO MMM, in which ZIF-8 particles are randomly dispersed into PEO matrix, the ZIF-8@PAN-4/PEO MMM with the same ZIF-8 loading of about 16.6 wt% presents enhanced CO 2 permeability and CO 2 /N 2 selectivity, which are increased by 52.4% and 44.3%, respectively. This is due to the continuous ZIF-8 transport pathway and good interfacial compatibility, which is also confirmed by the result of gas diffusivity and solubility coefficients. Together with the outstanding mechanical strength and stability, the proposed MMM with continuous ZIF-8 transport pathway paves a new way to improve CO 2 permeability.
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高影响因子
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