Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 10
·4485-4493
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IF 9.931
Lingyou Zeng,Kaian Sun,Zhichao Yang,Shengli Xie,Yanju Chen,Zhi Liu,Yaqing Liu,Jinchong Zhao,Yunqi Liu,Chenguang Liu
Three-dimensional (3D) nanomaterials have received significant attention for large-scale functional applications due to their large specific surface areas as well as desired electrical, physicochemical, and catalytic properties. Herein, we present a facile and effective synthetic route for in situ grown 3D hierarchical Ni3S2 superstructures (rod-like arrays and nanoforest patterns) on nickel foam. This handy strategy endows the Ni3S2 superstructures with large surface active areas, porosity, and macro-/mesoporous structures. We have shown that these materials can serve as highly active, binder-free, bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Moreover, these materials were found to provide a ∼100% faradaic yield towards both HER and OER and exhibit remarkable catalytic stability (for >50 h).
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Surfaces and Interfaces
·
2024
·
IF 5.7
Xinru Wang,Qiuxu Chen,Daming Yang,Ying Li,Dongxu Yin,Baoxin Ni,Wei Lu,Guiru Sun,Ming Feng
Photo-assisted electrochemical strategy has garnered interest for its ability to diminish the large overpotential of lithium-oxygen batteries (LOBs). Nonetheless, creating a sophisticated photocatalyst capable of absorbing a wide spectrum of light and dramatically lowering the recombination rate for electron-hole pairs presents a significant challenge. Herein, we design an Ag-doped ZnO (Ag@ZnO) hollow nanosphere as photocatalysts to boost the reaction dynamics of photo-assisted LOBs. The Ag@ZnO hollow nanospheres, featuring a mesoporous structure, are beneficial for improving O 2 transport and enabling the retention of discharge products. Additionally, the ability to absorb light and the efficiencies of electron-hole separation are enhanced for Ag@ZnO as a result of Ag doping. The electrons generated by photoexcitation facilitate the conversion of O 2 to produce Li 2 O 2 during discharge, whereas during charging, the presence of holes causes the decomposition of Li 2 O 2 . Consequently, a significantly low overpotential of 0.22 V, ultrahigh cycling efficiency of 93.73%, and good reversibility was achieved for the photo-assisted LOBs using Ag@ZnO. We consider that this work can offer a reliable strategy to improve electrochemical kinetics and contribute to the development of efficient photocatalysts for photo-assisted LOBs.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
·
IF 3.8
Yu-Zhen Xu,Yu-Le Wang,Yu-Dong Shan,Song-Hai Wu,Yong Liu,Xu Han
Selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) by O2 under solvent- and initiator-free conditions is a challenge in chemical processes, which is still constrained by its low selectivity (theoretical selectivity of 50.0%). Given the low epoxide selectivity (<20.0%) of single metal catalysts, we propose a relay catalysis strategy on the oxidation of Cy to Cy-ep with high selectivity by the spherical Mg–Mo bimetallic oxide (MMO). Such a relay catalyst exhibits a desirable Cy conversion of 31.0% and a high selectivity of 49.3% toward Cy-ep. Meanwhile, the high stability and reusability of MMO also indicate its potential to be used for industrial scale-ups. A series of characterizations and DFT calculations reveal that the negatively charged lattice oxygen in [MgII–O–II] adsorbs allylic H of Cy to weaken the bond energy of the allylic C–H bond and form Cy•, and then Cy• rapidly traps O2 to give CyOO•, which subsequently abstracts H from allylic C–H of another Cy to form 2-cyclohexene-1-hydroperoxide (Cy-OOH) and Cy•, achieving the propagation cycle. On the other hand, the Mo(VI) site in MMO catalyzes the produced Cy-OOH peroxo, which then oxidizes Cy to Cy-ep and 2-cyclohexene-1-ol. This work provides insight into the relay catalyst for the epoxidation of olefin with O2 with high selectivity under solvent- and initiator-free conditions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Bingbing He,Qinyuan Wang,Ying Chen,Weifeng Yao
The development of a cost-effective method for synthesizing hydrogen peroxide (H2O2) holds significant importance. Here, we introduce a novel catalyst, a nitrogen-doped carbon-loaded nickel nanoparticle catalyst (Nix NPs@N–C), tailored for efficient H2O2 production via the two-electron oxygen reduction reaction. Benefiting from the synergistic interplay between highly active nickel nanoparticles and nitrogen-doped carbon, the optimal Nix NPs@N–C catalyst demonstrates an outstanding 78% selectivity for H2O2 at 0.5 V vs a reversible hydrogen electrode (RHE), yielding approximately 387 mmol g–1 h–1 in a 0.1 M KOH alkaline solution at 0.3 V vs RHE. With its utilization of cost-effective raw materials, streamlined synthesis method, and exceptional catalytic performance, the Nix NPs@N–C catalyst emerges as a promising candidate for electrocatalytic H2O2 synthesis in practical applications.
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ACS Catalysis
·
2025
·
IF 13.1
Weina Yang,Yachao Wang,Yaxiong Wei,Guofeng Zhao,Weixin Huang,Cong Fu
Photocatalytic oxidative coupling of methane (OCM) offers a sustainable pathway for direct conversion of methane into value-added hydrocarbons, yet faces persistent challenges in balancing efficient methane activation with suppression of overoxidation. Here, we present a TiO2-based photocatalyst decorated with highly dispersed Ag–Co dual sites that achieves superior performance in continuous-flow OCM. The optimized AgCo–TiO2 system demonstrates a remarkable C2 hydrocarbon production rate of 1.7 mmol g–1 h–1 with 91% selectivity while maintaining stable operation for over 30 h. In situ spectroscopic analyses indicate that the introduced Co species induce mobile-charge imbalances, driving the directional transfer of photogenerated electrons and effectively suppressing electron–hole recombination. Coupled with Ag serving as a catalytic center, these effects synergistically enhance O2 activation, C–H bond cleavage, and selective C–C coupling, thereby contributing to the superior catalytic performance. This work provides valuable mechanistic insights into the photocatalytic OCM process, highlighting the pivotal role of precisely engineered charge transfer pathways in enabling efficient methane-to-C2 conversion.
研究领域:
光催化
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材料科学
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化学工程
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环境化学
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能量转换
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2021
·Vol. 105
·期 4
·2690-2701
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IF 3.784
Lu Zou,Zhao Lu,Ziling Wang,Bo Chi,Jian Pu
Developing high-efficiency and cost-effective bifunctional electrocatalysts toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is an urgent issue for the oxygen-based electrochemical devices. Herein, an interface engineering concept has been proposed to achieve high-performance Ag–PBSC (Ag–PrBa 0.5 Sr 0.5 Co 2 O 5+δ ) heterostructure nanofibers catalyst. Benefiting from the significant ligand action and interparticle cooperation of exsolved Ag NPs and PBSC double perovskite, ORR/OER catalytic kinetics have been successfully boosted. In details, the PBSC double perovskite possessing abundant oxygen vacancies can provide oxygen channels and facilitate the transfer of electrons and oxygen. The embedded Ag NPs can deliver superior catalytic durability for the heterostructure interface. As expected, the as-synthesized Ag-PBSC heterostructure catalyst performs a favorable electrochemical performance in the oxygen-based applications. In alkaline media, the catalyst exhibits an excellent activity for ORR ( E onset : 0.88 V vs. RHE and E 1/2 : 0.72 V vs. RHE) and OER (1.67 V at 10 mA cm –2 ). When adopting the Ag–PBSC heterostructure catalyst in LOBs, the corresponding battery provides an outperforming capacity performance (13 000 mAh g –1 ), low discharge–charge polarization (1.37 V), and considerable cycling performance (128 cycles at the restricted capacity of 3 000 mAh g –1 and 400 mA g –1 ). Apparently, the work described here confirms that the interface engineering of perovskites can open up opportunities to develop highly active and durable heterostructure electrocatalysts for multitudinous oxygen-based electrochemical applications.
研究领域:
材料科学
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电化学
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能源存储与转换
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Zaiyong Yang,Zhiheng Hao,Shunxin Zhou,Peng Xie,Zengxi Wei,Shuangliang Zhao,Fuzhong Gong
Direct synthesis of hydrogen peroxide (DSHP) from H2 and O2 offers a promising alternative to the present commercial anthraquinone method, but it still faces the challenges of low H2O2 productivity, low stability of catalysts, and high risk of explosion. Herein, by loading in a microchannel reactor, the as-synthesized Pd–Sn alloy materials exhibit high catalytic activity for H2O2 production, presenting a H2O2 productivity of 3124 g kgPd–1 h–1. The doped Sn atoms on the surface of Pd not only facilitate the release of H2O2 but also effectively slow down the deactivation of catalysts. Theoretical calculations demonstrate that the Pd–Sn alloy surface has the property of antihydrogen poisoning, showing higher activity and stability than pure Pd catalysts. The deactivation mechanism of the catalyst was elucidated, and the online reactivation method was developed. In addition, we show that the long-life Pd–Sn alloy catalyst can be achieved by supplying an intermittent flow of hydrogen gas. This work provides guidance on how to prepare high performance and stable Pd–Sn alloy catalysts for the continuous and direct synthesis of H2O2.
研究领域:
化学工程
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催化科学
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材料科学
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高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2021
·Vol. 46
·期 3
·2737-2747
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IF 5.164
Yueheng Fan,Aiming Wu,Xiaohui Yan,Shuiyun Shen,Zhang Junliang
Summary Both the activity and structure of a cathode, when it is used in non-aqueous Li-O 2 batteries, play a prominent role in the aspects of durability and capacity. In this work, α-MnO 2 /prGO hybrid nanocomposites with a three-dimensional (3D) porous structure are proposed to act as the cathode to improve the battery performance. Highly active α-MnO 2 /prGO nanocomposites with different mass ratios are synthesized through a two-step template method and a subsequent annealing process. It is found that the optimal 50% α-MnO 2 /prGO cathode exhibits outstanding discharge capacity of 13 294 mAh g −1 under the condition of 100 mA g −1 . Meanwhile, with the limited capacity and currency density of 1000 and 100 mA g −1 , respectively, the battery maintains excellent durability for 239 cycles. Significantly, it is clear that the excellent electrochemical performance of the nanocomposites is strongly associated with the synergistic effect of their distinct porous architecture and the ORR/OER catalytic activity.
研究领域:
材料科学
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电化学
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能源存储与转换
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Journal of the American Chemical Society
·
2014
·
IF 11.444
Xibin Pang,Wei Chang,Chuncheng Chen,Hongwei Ji,Wanhong Ma,Jincai Zhao
The molecules O2 and H2O dominate the cleavage of aromatic sp2 C–C bonds, a crucial step in the degradation of aromatic pollutants in aqueous TiO2 photocatalysis, but their precise roles in this process have remained elusive. This can be attributed to the complex oxidative species involved and to a lack of available models for reactions with a high yield of direct products. Here, we used oxygen-18 isotope labeled O2 and H2O to observe the aromatic ring-opening reaction of the model compound 3,5-di-tert-butylcatechol (DTBC), which was mediated by TiO2 photocatalysis in an aqueous acetonitrile solution. By analyzing the primary intermediate products (∼75% yield), especially the seven-membered ring anhydrides that were formed, we obtained direct evidence for the oxygen atom of dioxygen insertion into a C–C bond of the aromatic ring. This indicates that molecular oxygen is the ultimate ring-opening agent in TiO2 photocatalysis and that it undergoes single O atom incorporation rather than the previously proposed molecular oxygen 1,2-addition processes. The ratio of intradiol to extradiol products depends on the particle size of TiO2 catalysts used, which suggests that the O2 activation is correlated with the available coordination sites on the TiO2 surface in the photocatalytic cleavage of the aromatic ring.
研究领域:
环境科学
·
化学
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Shumin Li,Jun Tan,Zhejun Jiang,Jin Wang,Zhengquan Li
Dye-sensitized systems show promising in photocatalysis because they can separate the tasks of light absorption, charge generation and surface catalysis to two coupled components. In this system, it is crucial to develop suitable catalysts capable of receiving dye-injected charges and having high activity to a given reaction. Aiming to photocatalytic H 2 and O 2 production, we present a metal-organic framework derived route to prepare bimetallic Fe-Ni-P nanotubes using Fe-Ni-MIL-88 nanorods as templates. When integrated with different dyes, these Fe-Ni-P nanotubes can serve as efficient catalysts for photocatalytic H 2 and O 2 production, respectively. Additionally, catalytic activities of such dye-sensitized systems can be conveniently regulated by tailoring the metal compositions in Fe-Ni-P nanotubes. The photocatalytic H 2 production of Fe 1 -Ni 2 -P can reach 5420 μmol g cat −1 h −1 under eosin-Y sensitization, which is 24 times and 6.7 times higher than Fe 2 P and Ni 2 P, respectively. The photocatalytic O 2 production of Fe 1 -Ni 2 -P can reach 900.3 μmol g cat −1 h −1 under [Ru(bpy) 3 ]Cl 2 sensitization, about 4.6 times and 2.9 times higher than Fe 2 P and Ni 2 P. The roles of different components in the system have been explored and corresponding working mechanism is proposed. This work demonstrates a new type of dye-sensitized systems consisting of bimetallic phosphides and provides a facile route to regulate their photocatalytic performance.
研究领域:
材料科学
·
光催化
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FREE RADICAL BIOLOGY AND MEDICINE
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2018
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IF 6.02
Qing Li,Jie Su,Shi-Jie Jin,Wei Wei,Xiao-dong Cong,Xiao-Xue Li,Ming Xu
Background Insulin resistance in endothelial cells contributes to the development of cardiovascular disease in type 2 diabetes mellitus (T2DM). Therefore, there are great potential clinical implications in developing pharmacological interventions targeting endothelial insulin resistance. Our previous studies indicated that argirein which was developed by combining rhein with L -arginine by a hydrogen bond , could substantially relieved stress related exacerbation of cardiac failure and alleviated cardiac dysfunction in T2DM, which was associated with suppressing NADPH oxidase activity. However, it is unclear whether argirein treatment attenuates the vascular lesion and dysfunction in T2DM and its underlying mechanisms. Methods and results The rat aortic endothelial cells (RAECs) were used to treat with palmitic acid (PA), a most common saturated free fatty acid , which could induce insulin resistance. It was showed that argirein increased glucose uptake and glucose transporter-4 (Glut4) expression and reversed the phosphorylation of IRS-1-ser307 and AKT-ser473, consequently resulting in the increase of the production of eNOS and NO in PA-induced RAECs. We further found that argirein blocked the Nox4-dependent superoxide (O 2 -. ) generation, which regulated glucose metabolism in RAECs during PA stimulation. In vitro, argirein increased the release of endothelial NO to relieve the vasodilatory response to acetylcholine and insulin, and restored the expression of Nox4 and pIRS-1-ser307 in the aorta endothelium of high-fat diet (HFD)-fed rats following an injection of streptozocin (STZ). Conclusion These results suggested that argirein could improve endothelial insulin resistance which was attributed to inhibiting Nox4-dependent redox signaling in RAECs. These studies thus revealed the novel effect of argirein to prevent the vascular complication in T2DM.
研究领域:
药理学
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内分泌学
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心血管科学
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糖尿病研究
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高影响因子
ADVANCED MATERIALS
·
2026
·
IF 29.1
Da-Shuai Huang,Yi Tang,Pei-Qin Liao,Xiao-Ming Chen
Electrochemical CO 2 reduction must move beyond purified CO 2 to use real-world sources like flue gas or captured CO 2 . But such low-concentration feeds pose two problems: residual O 2 poisons the reaction, triggering competing oxygen reduction reaction, cutting carbon efficiency, and degrading the catalyst, while low CO 2 concentration limits mass transfer and conversion. We solve both with a kinetic molecular sieve: polyethylene glycol-coated bismuth nanoparticles (Bi@PEG). Under simulated flue gas (15% CO 2 , 5% O 2 , 80% N 2 ), Bi@PEG demonstrates record-breaking performance for CO 2 electroreduction to formate, achieving a Faradaic efficiency of 94.1 ± 0.6%, a current density of 0.91 A·cm −2 , and a single-pass CO 2 conversion of 72.5%, and maintains this performance even at 8% O 2 . Mechanism studies show the PEG layer selectively admits CO 2 (small size, quadrupole moment, strong Lewis acid, base interaction with ether oxygens; binding energy −27.4 kJ mol −1 ; diffusion barrier 0.57 eV), resulting in interfacial CO 2 enrichment. In contrast, O 2 transport is significantly impeded due to a higher diffusion barrier (0.83 eV), weak binding affinity (−3.0 kJ mol −1 ), and steric hindrance. By overcoming the dual challenges of low CO 2 concentration and oxygen interference, this work establishes “armored catalysis” as a universal approach for electrochemical CO 2 conversion using realistic, low-concentration, oxygen-containing carbon sources.
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