INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Chenxiao Wang,Kui Liu,Yinghao Wu,Guangjun Zhang,Xuelian Li,Jiaxin Wu,Ruili Sun,Ting Chen,Lang Xu,Shaorong Wang
A-site doping with Ca 2+ , Sr 2+ for the cobalt-free BaFeO 3-δ -based cathode materials for proton-conducting ceramic fuel cells (PCFCs) is studied. The composite Ba 0·8 Ca 0·2 FeO 3-δ (BCF0.2)-BaZr 0.1 Ce 0·7 Y 0.1 Yb 0.1 O 3-δ (BZCYYb) and Ba 0·8 Sr 0·2 FeO 3-δ (BSF0.2)-BZCYYb electrode show polarization resistance (R p ) of 0.156 Ω cm 2 and 0.308 Ω cm 2 at 700 °C, respectively. It is found that the Ca or Sr doping not only benefits oxygen vacancy formation and ion migration but also optimizes the surface oxygen reduction reaction (ORR) process. The density functional theory (DFT) calculations show that the Gibbs energies of *OOH and *OH intermediates are decreased, indicating an enhanced surface ORR. The PCFC with BCF0.2-BZCYYb composite cathode achieves the maximum power density of 299.75 mW cm −2 at 700 °C and shows good stability at 650 °C for 65 h under a constant voltage of 0.75 V. These findings suggest that the BCF0.2-BZCYYb has the potential to serve as cobalt-free cathode materials for PCFCs.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 35
·期 16
·2420014
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IF 18.5
Dongrong Yang,Qiye Guan,Baowen Wang,Da Zhang,Kun Ren,Huangkai Zhou,Xiaoyu Li,Yingjie Zhou,Yongqing Cai,Pan Liu,Lanqing Zhao,Minjie Hou,Bin Yang,Dongfeng Xue,Feng Liang
Solid-state sodium-metal batteries (SSSBs) have emerged as a potential next-generation energy storage technology due to their abundant resource, high energy density, and safety. However, the uncontrolled Na dendrite growth and low charging/discharging rate pose a severe constraint on their practical applications. Herein, high interfacial sodium-ion diffusion performance and interface stability of Na anode are achieved in SSSBs by designing an interfacial built-in electric field (IBEF) driven by a laminated hybrid solid electrolyte with a mixed-ion/electron-conducting layer. The electrochemical characterizations and density functional theory (DFT) calculations reveal that IBEF effectively improves interfacial sodium-ion diffusion by reinforcing electron delocalization and decreasing Na + transfer energy barrier. Furthermore, finite element simulation and experiments indicate that the IBEF endows a uniform interfacial charge distribution and Na deposition during plating/stripping. The IBEF boosts the cyclability of solid-state symmetric cells, enabling ultralong cycle life over 26 400 cycles at 0.1 mA cm −2 , the Na/Na 3 V 2 (PO 4 ) 3 (NVP) full cells display a remarkable capacity retention of 97.4% after 1500 cycles at 2.0 C and stable charging/discharging even at −20 °C. Na/NVP pouch cells exhibit a capacity of 65.7 mAh g −1 after 50 cycles under 0.19 mA g −1 .
研究领域:
材料科学
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电化学
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能源存储技术
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Shuangjiang Li,Yi Liu,Lan Shi,Tianding Hu,Mengrui Li,Churu Zhang,Shaoyun Shan,Yunfei Zhi
A Salen-functionalized ionic polymer (Zn-Salen-IP) was synthesized through a metal-assisted method. The structure and microstructure were characterized by using different characterization methods. Subsequently, the cycloaddition of CO 2 with epoxide was used to investigate the catalytic activity of Zn-Salen-IP. The relationship between the types of ions within Zn-Salen-IP and its catalytic performance was thoroughly explored. Single-factor investigations were used to determine the optimal reaction conditions for catalytic CO 2 cycloaddition used Zn-Salen-IP. The universality and recyclability of Zn-Salen-IP were systematically studied under the optimized conditions. Finally, Density functional theory calculations were employed to research the mechanism and pathway of the CO 2 cycloaddition reaction catalyzed by Zn-Salen-IP with dual functional active sites. This provided a deep understanding for the rate-determining step and the influence of the nucleophilicity of the halogen anion in cycloaddition reaction of CO 2 and epoxide.
研究领域:
化学工程
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材料科学
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环境科学
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Changjun Yang,Shuai Xu,Fanchang Peng,Wenyao Zhou,Quan Zhou,Xi Chen,Bingguang Zhang,Kejian Deng
The cis / trans isomeric effects of cobalt thioporphyrazine (CoPz) bearing 1,4-dithiin (A) and bis(butylthio) (B) groups on their photocatalytic performance were investigated by photocatalytic selective aerobic oxidation of 5-hydroxymethylfurfural (HMF) in aqueous solution under simulated sunlight. The results demonstrated that the cis -CoA 2 B 2 consistently showed higher photocatalytic activity than the trans -CoA 2 B 2 , especially in alkaline solution. Meanwhile, the cis -CoA 2 B 2 favored oxidizing HMF to 2,5-furandicarboxylic acid (FDCA), while the trans -CoA 2 B 2 preferred yielding 2,5-diformylfuran (DFF). Under alkaline conditions, the yield of FDCA can reach 73% with a selectivity of 95% in the presence of cis -CoA 2 B 2 after reacting 14 h, while 37% of DFF yield with a selectivity of 81% can be achieved in the presence of trans -CoA 2 B 2 after reacting 12 h. The relationship between the structure of cis / tr ans isomers and their photocatalytic performance was further explored by density functional theory (DFT) calculations. The active species originated from cis -CoA 2 B 2 and trans -CoA 2 B 2 were also examined by trapping experiments.
研究领域:
化学
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材料科学
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催化反应
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DOI
高影响因子
ACS Applied Nano Materials
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2022
·
IF 6.14
Ruiqi Liu,Juan Yang,Rui Liu,Yumeng Tang,Lijin Huang,Qin Shuai
Covalent organic frameworks (COFs) featuring long-range ordered pore size and large specific surface area have been recognized as a fantastic platform for contaminant removal. However, the influence of nanopore size on their adsorption behavior has not been well understood. Herein, three stable β-ketoenamine COFs, i.e., TpPa-1, TpBD, and TpTph, with the same type of linkage but diverse nanopore size were successfully obtained by a salt-mediated crystallization strategy. Their adsorption behavior and interaction mechanisms toward sulfamerazine (SMR) in aqueous solution were studied by adsorption experiments and density functional theory (DFT) calculations. The adsorption kinetics of SMR over COFs followed the order TpPa-1 < TpBD < TpTph, which is consistent with the changing trend of nanopore size, suggesting that a large nanopore is beneficial in boosting mass transfer. However, the maximum adsorption capacities followed the order TpPa-1 (82.9 mg/g) < TpTph (150 mg/g) < TpBD (188 mg/g). Referring to the data of specific surface area and nanopore size of COFs, it can be inferred that the specific surface area of COFs plays a less important role, and pore characteristics might be the dominant factor affecting the adsorption behavior of SMR. Furthermore, DFT results confirmed that SMR can be loaded into the channels of TpPa-1, TpBD, and TpTph due to its small molecule size, and the adsorption interactions are dominated by C–H···π and H-bonding. The different adsorption performance of SMR on TpPa-1, TpBD, and TpTph stems from their different number of adsorption sites and binding energies. These findings demonstrated the feasibility of adjusting the adsorption capacity of COFs by regulating the nanopore sizes, providing possible solutions for tailor-made COFs with superior adsorption performance.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2023
·Vol. 25
·期 37
·25116-25121
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IF 3.3
Min Kou,Young-Ho Oh,Sungyul Lee,Xianglei Kong
We present the origin of the observed differentiation of lactose and lactulose achieved by complexation with sodiated L-arginine (ArgNa+). We find that the infrared multiphoton dissociation (IRMPD) bands in 3600–3650 and >3650 cm−1 regimes for gas phase lactose and lactulose, respectively, vanish when forming host–guest complexes with ArgNa+. We interpret these differences in the IRMPD spectra by scrutinizing the interactions between the functional groups (guanidium, –CO2−Na+) in ArgNa+ and –OHs in lactose/lactulose. Our calculated structures and infrared spectra of lactose/ArgNa+ and lactulose/ArgNa+ host–guest pairs indicate that the functional groups interact with the low- and high-frequency –OH stretch modes of lactose and lactulose, respectively, in the 3600–3720 cm−1 window.
研究领域:
化学
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生物化学
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光谱学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Song Zou,Guichun He,Xinyang Yu,Hong Zhong
Three novel dithiocarbamate surfactants including 2-hydroxypropyl diethyldithiocarbamate (HPD-2), 3-hydroxypropyl diethyldithiocarbamate (HPD-3), and 2-(2-hydroxyethoxy)ethyl diethyldithiocarbamate (HED-2) were prepared and characterized by FTIR, 1 H/ 13 C NMR and HRMS. They were first employed as collectors to float chalcopyrite. DFT calculations were performed to anticipate the structure–reactivity of the novel dithiocarbamates, revealing that the reaction sites were primarily distributed in C S and OH groups. Compared with HPD-2 and HPD-3, HED-2 possessed a higher chemical reactivity owing to the C-O-C group. Microflotation results indicated that the collecting ability of the three dithiocarbamate collectors towards chalcopyrite followed as HPD-3 > HED-2 > HPD-2. FTIR and XPS demonstrated that HED-2 chemisorbed onto the surface of chalcopyrite through newly generated Cu S and Cu O bonds.
研究领域:
矿物加工工程
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理论化学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Bin Chen,Dehuan Shi,Renxia Deng,Xin Xu,Wenxia Liu,Yang Wei,Zheyuan Liu,Shenghong Zhong,Jianfeng Huang,Yan Yu
Revealing the synergistic catalytic mechanism involving multiple active centers is crucial for understanding multiphase catalysis. However, the complex structures of catalysts and interfacial environments pose a challenge in thoroughly exploring the experimental evidence. This study reports the utilization of a CuNi dual-atom catalyst (Cu/Ni–NC) for the electrochemical reduction of CO2. It demonstrates a high Faradaic efficiency of CO exceeding 99%, remarkable reaction activity with a partial current density surpassing –300 mA cm–2, and prolonged stability for more than 5 days at a current density of –200 mA·cm–2. Operando characterization techniques and density functional theory calculations reveal that Ni atoms function as active sites for the activation and hydrogenation of CO2, while Cu atoms serve as active sites for the dissociation of H2O, supplying protons for the subsequent hydrogenation process. Moreover, the electronic interactions between Ni and Cu atoms facilitate the formation of *COOH and the dissociation of H2O, illustrating a synergistic reduction of CO2 at the dual-atom sites.
研究领域:
材料科学
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电化学
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理论计算
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 21
·7529-7536
·
IF 9.48
Huihuang Chen,Xu Guo,Xiangdong Kong,Yulin Xing,Yan Liu,Bolong Yu,Qun-Xiang Li,Zhigang Geng,Rui Si,Jie Zeng
CO2 electroreduction into valuable products holds great promise for energy supply and environmental remediation but remains a challenge due to the lack of high-performance electrocatalysts. Herein, we developed an efficient strategy to prepare highly active Fe single-atom catalysts (Fe–N5/Fe–N6) by tuning the coordination number of Fe with N towards CO2 electroreduction. The faradaic efficiency of CO for Fe–N5 exceeded 90% ranging from −0.35 to −0.65 V versus the reversible hydrogen electrode (vs. RHE) towards CO2 electroreduction. The turnover frequency of CO for Fe–N5 reached 5006 h−1 at −1.05 V vs. RHE, which was 3.8 times that (1324 h−1) of Fe–N6. Besides, CO was generated at an overpotential as low as 50 mV over Fe–N5, smaller than that (90 mV) over Fe–N6. Density functional theory calculations demonstrated that Fe–N5 facilitated the adsorption and activation of CO2 to form the *COOH intermediate, thus leading to superior selectivity and activity for CO2 electroreduction.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qi Si Chen,Peng Lei Cui,Jun Yang,Dong Chen,Hui Liu,Huiyan Feng,Panagiotis Tsiakaras,Pei Kang Shen
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is regarded as an effective strategy to store abundant renewable energy and build a carbon neutral society. Gold (Au) and silver (Ag)-based catalysts for the effective electrochemical transformation of CO 2 to CO emerge as promising candidates. Heterogeneous nanocomposites composed of noble metals and semiconductors exhibit great potential for electrocatalytic CO 2 reduction through the electronic coupling effect at coherent interfaces. Herein, we successfully synthesize heterogeneous Ag 2 S-Au composite nanoparticles (NPs) as effective catalysts for CO production through CO 2 RR. At −0.8 V vs RHE, the heterogeneous Ag 2 S-Au nanocatalysts display a considerable CO Faradaic efficiency of 94.5%, and an appreciable CO partial current density of 9.17 mA cm −2 . Moreover, they exhibit good stability for 30 h without obvious decrease. On the basis of density functional theory (DFT) calculations, it can be made clear that the heterogeneous Ag 2 S-Au interface is energetically more beneficial to the generation of COOH* intermediate for CO 2 RR. This study provides a new application for noble metal–semiconductor nanocomposites.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Jieding Wei,Renqiang Zhao,Dian Luo,Xiangyu Lu,Wenxiu Dong,Yucheng Huang,Xiaomei Cheng,Yonghong Ni
Much effort has been devoted to improving the photocatalytic capacity of graphitic carbon nitride (g-C 3 N 4 ). In this paper, we reported the successful synthesis of a hybrid photocatalyst with superb photocatalytic hydrogen production activity through decorating atomically precise Ni 6 (SC 2 H 4 Ph) 12 nanoclusters on g-C 3 N 4 nanosheets (labeled as Ni 6 /g-C 3 N 4 ) at room temperature. Zeta potential experiments demonstrated that the electrostatic interaction between Ni 6 and g-C 3 N 4 led to the formation of Ni 6 /g-C 3 N 4 . The photocatalytic measurements revealed that the 5 %-Ni 6 /g-C 3 N 4 prepared with the original mass ratio of m(Ni 6 )/m(g-C 3 N 4 ) = 1/20 exhibited the strongest hydrogen production activity. In the system with triethanolamine (TEOA) as the sacrifice agent, the visible-light hydrogen production rate reached up to 5.87 mmol h −1 g −1 , approximately 290 times higher than that of pure g-C 3 N 4 (0.02 mmol h −1 g −1 ). Density functional theory (DFT) calculations testified that the above significant enhancement of photocatalytic hydrogen evolution of the hybrid photocatalyst arose from the photogenerated electrons transfer from Ni 6 to g-C 3 N 4 .
研究领域:
材料科学
·
催化化学
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理论计算
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产品关联
DOI
PubMed
高影响因子
Processes
·
2022
·Vol. 10
·期 9
·1815
·
IF 3.352
Yao Ma,Haoliang Li,Chunsheng Xie,Xiaodong Du,Xueqin Tao,Guining Lu
Soil-washing is a potential technology for the disposal of soil contaminated by e-waste; however, the produced soil-washing effluent will contain polybrominated diphenyl ethers (PBDEs) and a large number of surfactants, which are harmful to the environment, so the treatment of PBDEs and the recycling of surfactants are the key to the application of soil-washing technology. In this study, coconut shell granular-activated carbon (GAC) was applied to remove PBDEs from Triton X-100 (TX-100) surfactant which simulates soil-washing effluent. The adsorption results show that, GAC can simultaneously achieve effective removal of 4,4′-dibromodiphenyl ether (BDE-15) and efficient recovery of TX-100. Under optimal conditions, the maximum adsorption capacity of BDE-15 could reach 623.19 μmol/g, and the recovery rate of TX-100 was always higher than 83%. The adsorption process of 4,4′-dibromodiphenyl ether (BDE-15) by GAC could best be described using the pseudo-second-order kinetic model and Freundlich isothermal adsorption model. The coexistence ions had almost no effect on the removal of BDE-15 and the recovery rate of TX-100, and the solution pH had little effect on the recovery rate of TX-100; BDE-15 had the best removal effect under the condition of weak acid to weak base, indicating that GAC has good environmental adaptability. After adsorption, GAC could be regenerated with methanol and the adsorption effect of BDE-15 could still reach more than 81%. Density functional theory (DFT) calculation and characterization results showed that, Van der Waals interaction and π–π interaction are dominant between BDE-15 and GAC, and hydrogen bond interactions also exist. The existence of oxygen-containing functional groups is conducive to the adsorption of BDE-15, and the carboxyl group (-COOH) has the strongest promoting effect. The study proved the feasibility of GAC to effectively remove PBDEs and recover surfactants from the soil-washing effluent, and revealed the interaction mechanism between PBDEs and GAC, which can provide reference for the application of soil-washing technology.Keywords:granular-activated carbon;polybrominated diphenyl ethers;Triton X-100;soil-washing effluent;adsorption;density functional theory calculation
研究领域:
环境科学
·
化学工程
✓ 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）