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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DOI
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Shuyu Wang,Miaomiao Cheng,Shenghui Wang,Wei Jiang,Feifei Yang,Xiaomei Shen,Lirong Zhang,Xiyun Yan,Bing Jiang,Kelong Fan
Radiotherapy (RT), essential for treating various cancers, faces challenges from tumor hypoxia, which induces radioresistance. A tumor-targeted “prosthetic-Arginine” coassembled nanozyme system, engineered to catalytically generate nitric oxide (NO) and oxygen (O 2 ) in the tumor microenvironment (TME), overcoming hypoxia and enhancing radiosensitivity is presented. This system integrates the prosthetic heme of nitric oxide synthase (NOS) and catalase (CAT) with NO-donating Fmoc-protected Arginine and Ru 3+ ions, creating HRRu nanozymes that merge NOS and CAT functionalities. Surface modification with human heavy chain ferritin (HFn) improves the targeting ability of nanozymes (HRRu-HFn) to tumor tissues. In the TME, strategic arginine incorporation within the nanozyme allows autonomous O 2 and NO release, triggered by endogenous hydrogen peroxide, elevating NO and O 2 levels to normalize vasculature and improve blood perfusion, thus mitigating hypoxia. Employing the intrinsic O 2 -transporting ability of heme, HRRu-HFn nanozymes also deliver O 2 directly to the tumor site. Utilizing esophageal squamous cell carcinoma as a tumor model, the studies reveal that the synergistic functions of NO and O 2 production, alongside targeted delivery, enable the HRRu-HFn nanozymes to combat tumor hypoxia and potentiate radiotherapy. This HRRu-HFn nanozyme based approach holds the potential to reduce the radiation dose required and minimize side effects associated with conventional radiotherapy.
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DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2022
·Vol. 34
·期 40
·2201838
·
IF 32.086
Guiru Sun,Rui Gao,Hailiang Jiao,Dan Luo,Yan Wang,Zexu Zhang,Wei Lu,Ming Feng,Zhongwei Chen
The major challenges for Li-O 2 batteries are sluggish reaction kinetics and large overpotentials due to the cathode passivation resulting from insulative and insoluble Li 2 O 2 . Here, a novel nanodot (ND)-modified electrolyte is designed by employing cobalt bis(trifluoromethylsulfonyl)imide (Co(TFSI) 2 ) as an electrolyte additive. The Co(TFSI) 2 additive can react with discharge intermediate LiO 2 and product Li 2 O 2 to form CoO NDs. The generated CoO NDs are well dispersed in electrolyte, which integrates both the high catalytic activity of solid catalyst and the good wettability of soluble catalyst. Under the catalytis of CoO NDs, Li 2 O 2 is produced and deposits on the cathode together with them. At the recharge process, these well dispersed CoO NDs help to decompose solid Li 2 O 2 at a lower overpotential. The Li-O 2 cells with Co(TFSI) 2 exhibit a long cycle life of 200 cycles at a current density of 200 mA g −1 under a cutoff capacity of 1000 mAh g −1 , as well as a superior reversibility associated with the Li 2 O 2 formation and decomposition. The study is expected to broaden the range of electrolyte additives and provide a new view to developing highly dispersed NDs-based catalysts for Li-O 2 batteries.
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高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Yiqiao Wang,Siyuan Pan,Yong Guo,Shichao Wu,Quan-Hong Yang
Li-O 2 batteries require catalysts to solve the problem of sluggish oxygen-related reaction kinetics. However, the solid catalysts and redox mediators are intrinsically deficient due to poor solid contacts and shuttle problems, respectively. Here, we report lithium phthalimide-N-oxyl (LiPINO) as a phase transfer catalyst (PTC) for promoting Li 2 O 2 formation and its reversible decomposition through the solution-phase reactions. The interaction between LiPINO and oxygen species in the electrolyte enables the high dissolution and stability of oxygen species, the fast charge transfer at liquid-solid interfaces and superior kinetics, and the suppressed side reactions. The efficient bidirectional catalytic activity and high stability of LiPINO capacitate batteries with a highly improved discharge capacity (11400 mAh g −1 ), a largely lowered charge potential (3.14 V) and an extended cycle life (more than 200 cycles) both in O 2 and air. Our understanding of the phase-transfer catalysis towards the Li-O 2 electrochemistry and the discovery of the PTC with superior activity and stability provide deep insights into the design of the most reliable catalysts for Li-O 2 batteries.
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高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
Dongxiao Wang,Shuyin Xu,Jianlin Wang,Xiaohui Rong,Feiyu Zhou,Lifen Wang,Xuedong Bai,Bingan Lu,Chengjun Zhu,Yuesheng Wang,Yong-sheng Hu
Room-temperature Na-ion batteries have attracted great interest for over a decade owing to their natural abundance and similar intercalation chemistry with Li-ion. However, due to the uncontrolled decomposition of electrolyte and formation of solid electrolyte interphase, the large majority of sodium anode materials exhibit extremely low initial Coulombic efficiency and unsatisfactory cycling stability. Here we introduce a novel layered material, P2-Na 0.547 [M g 0.25 M n 0.75 ]O 2 , as an SEI-free negative electrode. This material, delivers a reversible capacity of 126 mAh g −1 with a high initial Coulombic efficiency of 108%, and capacity retention of ∼80% after 1000 cycles at 4C rate. Pairing with Na 3 V 2 (PO 4 ) 3 cathode, excellent rate performance of ∼60% capability at 15C, and extra-high initial Coulombic efficiency of 97% are achieved, all attributed to the SEI-free feature of Na 0.547 [M g 0.25 M n 0.75 ]O 2 . These results demonstrate the practical potential of our SEI-free anode material for high-power and long-life Na-ion batteries.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
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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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Chaofan Zhang,Qiu Zhuang,Hao Wang,Xintong Ying,Ruoyang Ji,Daohu Sheng,Wei Dong,Aming Xie
Hexavalent chromium (VI) heavy metal contamination is considered a serious threat to human health and the environment. The photocatalytic reduction of Cr(VI) basically occurs in the acidic environment, severely limiting the application of photocatalysts for the reduction of Cr(VI). Therefore, we designed a microenvironment strategy to achieve efficient reduction of Cr (VI) under neutral conditions by introducing sulfonic acid onto the aromatic conjugated skeleton. A series of characterizations and experiments have shown that the sulfonated aromatic ring conjugated polymer (Arcp-SO 3 H) can efficiently remove Cr(VI) under neutral or even alkaline conditions. In neutral solutions, Arcp-SO 3 H has a rate constant of 0.054 min −1 within 90 min and has an efficiency of nearly 100 %, which is 16 times faster than before sulfonation (k = 0.0316 min −1 ). the Arcp-SO 3 H surpasses all organic polymers and most metal-based photocatalysts in the related field. The capture experiments have proved that •O 2 – is the main role of reducing Cr(VI), and e - is secondary, which is quite different from the mechanism reported in the previous literature. The efficiency of reducing Cr (VI) in the four-cycle experiment is still 96 %, which also proves that Arcp-SO 3 H has strong stability and reproducibility. Thus, Arcp-SO 3 H has great practical application potential in the treatment of wastewater, and microenvironmental strategies also offer new possibilities in the field of environmental remediation.
研究领域:
环境科学
·
材料科学
·
化学工程
·
水处理技术
·
光催化
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·Vol. 13
·期 6
·120354
·
IF 7.2
Dan Dang,Xinyi Jiang,Juncheng Zhang,Yichao Wu,Baoxin Zha,Yingying Zhao
The valorization of crude glycerol, a major byproduct of biodiesel production, into high-value chemicals is critical for sustainable biorefineries. Herein, we report a novel alkali-free and homogeneous photocatalytic strategy for selectively converting glycerol to glycolic acid (GLYA) and formic acid (FA) using H 2 O 2 as a radical initiator under 365 nm UV irradiation. By optimizing volume fraction of H 2 O 2 (3.18％), light intensity (10 W), and temperature (35 °C), 99.3 % glycerol conversion with 23.47 % GLYA yield and 22.66 % FA yield was achieved within 2 h at ambient pressure. Crucially, scavenging experiments, post-illumination reactivity studies and the electron paramagnetic resonance (EPR) spectra revealed a synergistic •OH /•O 2 ⁻/ 1 O 2 radical cycle triggered by H 2 O 2 photolysis: (1) •OH initiates glycerol oxidation to glyceraldehyde; (2) •O 2 ⁻ (generated from O 2 reduction or H 2 O 2 decomposition) produces 1 O 2, which drives selective C-C cleavage to GLYA; (3) •OH/•O 2 ⁻/ 1 O 2 cycle enables mutual regeneration of active species, sustaining oxidation even after light cessation. This autocatalytic cycle eliminates the need for strong bases or noble metals, offering a green, energy-efficient route for glycerol upcycling.
研究领域:
催化化学
·
绿色化学
·
可再生能源
·
环境科学
·
化学工程
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
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
·
催化科学
·
材料科学
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2021
·Vol. 46
·期 3
·2737-2747
·
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
·
电化学
·
能源存储与转换
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高影响因子
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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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
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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高影响因子
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