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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Uncovering the Influence Mechanisms of H2O, O2, and NO2 on CeNiCa Dual-Function Material for Integrated CO2 Capture and In Situ Methanation

Linjia Li,Yiran Zhang,Jiaqi Feng,Shu Zhao,Wei Qiu,Ke Li,Zhen Huang,He Lin

Derived from carbon capture, utilization, and storage (CCUS), integrated carbon capture and utilization (ICCU) has been widely developed recently. Understanding the influences of H2O, O2, and NO2 on dual-function materials (DFMs) performance is crucial for their practical application. In this study, the influence mechanisms of O2, H2O, and NO2 on CeNiCa DFM for ICCU-methanation are investigated. The catalyst was oxidized by O2, H2O, and NO2. NO2 competes with CO2 for basic adsorption sites, inhibiting CO2 adsorption and methanation, but adsorbed NO2 is reduced mainly to N2 and NH3 during methanation. H2O induces agglomeration of the adsorbent and catalyst─the former due to the Ca(OH)2 mobility, and the latter attributed to OH-promoted migration and agglomeration of Ni. On this basis, it is proposed that the dominant roles of H2O, O2, and NO2 change in two- and multi-interference components, but the joint effects among them should not be neglected.

研究领域: 化学工程 · 环境科学
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JOURNAL OF CATALYSIS · 2024 · IF 6.5

Unveiling the significant promoting effect of SO2 on Ir/SiO2 catalyst for the CO-SCR of NOx in the presence of O2

Ruoyuan Li,Aixia Li,Junhua Li,Yao Wang,Zhiming Liu

Selective catalytic reduction of NO x by CO (CO-SCR) in the presence of O 2 is challenging because in this process CO is prone to being oxidized by O 2 , thus inhibiting NO x reduction by CO. Furthermore, SO 2 typically leads to the deactivation of the CO-SCR catalyst. Herein, a significant promoting effect of SO 2 on Ir/SiO 2 catalyst for the CO-SCR of NO x in the presence of O 2 is reported. In-situ X-ray Absorption Fine Structure (XAFS) and X-ray photoelectron spectroscopy (XPS) analysis showed that SO 2 does not affect the chemical nature of Ir 0 under reaction conditions. However, SO 2 can be oxidized to sulfate and deposit on the catalyst surface. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis demonstrated that the presence of SO 2 can inhibit the CO + O 2 reaction, thus leaving more CO available to reduce NO x over the active Ir 0 sites. As a result, the reduction of NO x is remarkably promoted even in the presence of O 2 and SO 2 .

CAS / MDL: 10025-83-9
研究领域: 催化化学 · 环境科学
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Bioactive Materials · 2024 · IF 18

Dual-layer microneedles with NO/O2 releasing for diabetic wound healing via neurogenesis, angiogenesis, and immune modulation

Changjiang Liu,Kun Liu,Dong Zhang,Yuting Liu,Yifeng Yu,Haifei Kang,Xianzhen Dong,Honglian Dai,Aixi Yu

Diabetic wounds present multiple functional impairments, including neurovascular dysregulation, oxidative imbalance, and immune dysfunction, making wound healing particularly challenging, while traditional therapeutical strategies fail to address these complex issues effectively. Herein, we propose a strategy utilizing dual-layer microneedles to deliver therapeutic gases by modulating neurovascular coupling and immune functions for diabetic wound treatment. The microneedle can respond to reactive oxygen species (ROS) in the diabetic microenvironment and subsequently generate oxygen (O 2 ) and nitric oxide (NO). These gases comprehensively promote neuro-vascular regeneration, reduce oxidative stress levels, and attenuate inflammation. In vivo studies demonstrate that the microneedle can accelerate diabetic wound healing by modulating neurovascular regeneration and inflammatory processes. Transcriptomic analyses further validate the involvement of related advantageous signaling pathways. The potential mechanism involves the activation of the PI3K-AKT-mTOR pathway to facilitate autophagy, ultimately accelerating the healing process. Thus, our multifunctional dual-layer microneedles provide an effective strategy for treating diabetic wounds.

研究领域: 生物医学工程 · 药理学 · 伤口愈合 · 糖尿病研究 · 神经科学 · 免疫学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2016 · IF 5.393

Mechanisms of Elemental Mercury Transformation on α-Fe2O3(001) Surface from Experimental and Theoretical Study: Influences of HCl, O2, and SO2

Ting Liu,Lucheng Xue,Xin Guo,Jia Liu,Yu Huang,Chuguang Zheng

The reaction mechanisms of a mixture gas of HCl, O2, and SO2 in Hg0 adsorption on α-Fe2O3(001) surface are clarified by a group of adsorption experiments and theoretical calculations based on the density functional theory. The role of O2 in removing Hg0 is greatly influenced by the reaction temperature, meanwhile, the O atom coverage could affect the adsorption performance of Hg0. The dissociated O2 competes with the active sites of Cl species on Fe surface at low temperature, however, at medium temperature HCl and O2 could simultaneously facilitate the Hg0 transformation. Combined with the theoretical calculations, the role of SO2 and the probable pathways in removing Hg0 are discussed. Lower concentration of SO2 as well as HCl could dissociate on α-Fe2O3(001) surface, and the intermediates combine with gaseous Hg0, forming mercury–sulfur, mercury–chlorine compounds, and so forth. In addition, the different concentrations of SO2 are also discussed, and the corresponding X-ray photoelectron spectroscopy analysis on contrasted samples is conducted to research the morphological characterization, providing a reliable basis for judging the probable pathways of Hg0 transformation.

CAS / MDL: 1309-37-1
研究领域: 环境科学 · 化学
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CHEMOSPHERE · 2022 · IF 8.943

Micro-polluted water resources treatment by PVDF-TiO2 membrane combined with Fe2+/sodium dithionite (DTN)/O2 pre-oxidation process

Wanying Xie,Wei Song,Ji Li,Xiaolei Zhang,Wenyi Dong,Feiyun Sun

Modifying PVDF membrane by blending hydrophilic nano TiO 2 has been highly concerning, but its practical application is not well investigated. In this study, PVDF-TiO 2 membrane was employed in two modes to treat micro-polluted raw water for the first time, direct membrane filtration and pre-oxidation assists membrane filtration. At two filtration modes, the PVDF-TiO 2 membrane had comparable rejection capability to the unmodified PVDF membrane, as the removal of permanganate index (COD Mn ) was 0.26–0.72 mg/L, UV 254 was 0.0070–0.0618 cm −1 , turbidity was 1.60–4.49 NTU, and the total number of colonies was 360–23,780 CFU/mL. As for raw water treatment , using Fe 2+ /sodium dithionite (DTN)/O 2 system as the pre-oxidation process to assist the filtration of the PVDF-TiO 2 membrane was feasible. After optimization, the applicable conditions of the Fe 2+ /DTN/O 2 process were DTN dosage at 100 mg/L and a C Fe / C DTN of 1:4. As a result, the effluent qualities of the PVDF-TiO 2 membrane significantly improved. It was investigated that atrazine (ATZ), COD Mn , UV 254, and turbidity reduced, which was realized by the synergic effects of the pre-oxidation by free radicals and flocculation by iron. Pre-oxidation of the Fe 2+ /DTN/O 2 process could also enhance the permeability of the PVDF-TiO 2 membrane from 53.6 to 58.0 L/(m 2 ·h), nearly two times the PVDF membrane. Besides, the practical fouling of the PVDF-TiO 2 membrane was stably alleviated by the reduced R t , R re, and R ir , mainly due to constraining the internal pore fouling effectively.

研究领域: 环境科学 · 水处理工程
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

Boosting the oxidative capacity of the Fe(0)/O2 system via an air-breathing cathode

Zhenchao Lei,Ziyuan Huang,Yimin Lin,Yuwei Liu,Zhang Yan,Wenxiao Zheng,Huanxin Ma,Zhi Dang,Chunhua Feng

The corrosion of Fe(0) in the presence of O 2 in nature can lead to the oxidation of organic compounds, but the efficiency is very limited. Herein, attempts were made to establish a galvanic system that separates the anodic Fe(0) oxidation reaction and the cathodic O 2 reduction reaction using an air-breathing cathode. Compared with the chemical Fe(0)/O 2 system, it exhibited a substantially higher capability of destroying a variety of pollutants, such as organic dyes (12 types), phenol , nitrobenzene , acetaminophen, phenol, and ethylenediaminetetraacetic acid. The degradation rate constant of a model dye (i.e., Rhodamine B) increased from 0.047 min − 1 (chemical) to 1.412 min −1 (galvanic) under the passive air-breathing condition. The electric circuit design promoted Fe(0) dissolution to Fe(II) and triggered electron transfer that drives O 2 reduction to H 2 O 2 , two important species responsible for the generation of HO • at high abundance. In addition, the galvanic Fe(0)/O 2 system produces electricity while destroying pollutants. Tests with real Ni plating wastewater further demonstrated the capability of the system to oxidize complexed organics and phosphite. This study provides a new strategy for boosting the oxidative capacity of the Fe(0)/O 2 system, which shows promise for acid wastewater treatment .

研究领域: 环境科学 · 化学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Co3O4–CuCoO2 Nanomesh: An Interface-Enhanced Substrate that Simultaneously Promotes CO Adsorption and O2 Activation in H2 Purification

Junfang Ding,Liping Li,Haorui Zheng,Ying Zuo,Xiyang Wang,Huixia Li,Shaoqing Chen,Dan Zhang,Xingliang Xu,Guangshe Li

Nanomaterials are widely used as redox-type reaction catalysts, while reactant adsorption and O2 activation are hardly to be promoted simultaneously, restricting their applications in many important catalytic fields such as preferential CO oxidation (CO-PROX) in H2-rich stream. In this work, an interface-enhanced Co3O4–CuCoO2 nanomesh was initially synthesized by a hydrothermal process using aluminum powder as a sacrificial agent. This nanomesh is systematically characterized by powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N2 adsorption, X-ray photoelectron spectroscopy, UV–vis absorption spectroscopy, Raman spectroscopy, X-ray absorption near-edge spectroscopy, hydrogen temperature-programmed reduction, and oxygen temperature-programmed desorption. It is demonstrated that the nanomesh possesses high-density nanopores, enabling a large number of CO adsorption sites exposed to the surface. Meanwhile, electron transfer from O2– to Co3+/Co2+ and the weakened bonding strength of Co–O bond at surfaces promoted the oxygen activation and redox ability of Co3O4. When tested as a catalyst for CO-PROX, this nanomesh with an optimized pore structure and a surface electronic structure, exhibits a strikingly high catalytic oxidation activity at low temperatures as well as a broader operation temperature window (i.e., CO conversion >99.0%, 100–200 °C) in the CO selective oxidation reaction. The present finding should be highly useful in promoting the quest for better CO-PROX catalysts, a hot topic for proton exchange membrane fuel cells and automotive vehicles.

CAS / MDL: 7429-90-5
研究领域: 催化材料 · 能源化学 · 燃料电池
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Catalysts · 2021 ·Vol. 11 ·期 1 ·82 · IF 4.146

Promoting Photoelectrochemical Water Oxidation on Ti-Doped Fe2O3 Nanowires Photoanode by O2 Plasma Treatment

Chuang Li,Dan Wang,Jiangli Gu,Yichun Liu,Xintong Zhang

Surface electron traps on semiconductor photoanodes mediate surface recombination and deteriorate the photoelectrochemical (PEC) water oxidation performance of the photoanode. Developing convenient methods to reduce surface electron traps is therefore essential for high efficiency PEC water oxidation on semiconductor photoanodes, particularly for nanostructured photoanodes with large surface area. Herein, we employ a O2plasma treatment to boost the PEC water oxidation performance of Ti-doped Fe2O3(Ti-Fe2O3) nanowires photoanodes, aiming to reduce surface oxygen vacancies, the dominant electron traps on Ti-Fe2O3surface. X-ray diffraction (XRD), scanning electron microscopy and spectroscopic analyses show that the oxygen plasma treatment changes the structural, morphological and optical properties negligibly, but it does reduce the content of surface oxygen vacancies, as estimated from O1s X-ray photoelectron spectroscopy spectra. An optimal O2plasma treatment (200 W, 70 s) increases the photocurrent density of the Ti-Fe2O3nanowire photoanode to 2.14 mA·cm−2(1.23 V vs. RHE) under air mass 1.5G simulated solar light, which is 1.95 times higher than the pristine Ti-Fe2O3nanowire photoanode. The surface hole transfer efficiency is also improved by 1.66 times due to the reduced surface recombination. The work suggests that O2plasma treatment is a convenient but effective method to boost the PEC water oxidation performance of Ti-Fe2O3photoanode and might be applicable to other semiconducting oxide photoanodes for high efficiency PEC water splitting.Keywords:photoelectrochemical water splitting;O2plasma treatment;surface oxygen vacancies;Ti-doped hematite nanowire arrays

研究领域: 材料科学 · 能源科学
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ChemElectroChem · 2018 ·Vol. 5 ·期 13 ·1702-1707 · IF 4.446

Super P Carbon Modified Lithium Anode for High-Performance Li−O2 Batteries

Jiaqi Wang,Junxiang Liu,Yichao Cai,Fangyi Cheng,Zhiqiang Niu,Jun Chen

Graphical Right off the batt : A Li@Super P composite anode with a high specific surface area is fabricated through a low-cost brushing method, which effectively decreases the interface impedance and overpotential of Li depositing/stripping. The anode can also mitigate the detrimental shuttling effect of I 3 − generated from LiI during the charging process. The combination of the protected Li anode and LiI mediator delivers superior Li−O 2 battery performance. Rechargeable Li−O 2 batteries represent a highly attractive battery technology, owing to a high theoretical energy density of 3500 Wh kg −1 , but they suffer from large charging polarization and lithium anode degradation on cycling. Herein, we report a Li−O 2 battery system with reduced polarization and a long lifespan, which is realized by using a novel Li@Super P composite anode integrated with lithium iodide in ether-based electrolyte. Coating a Super P carbon layer, with an optimal thickness of approximately 30 μm, onto the lithium anode results in a lowered interface impedance and a decreased Li depositing/stripping overpotential (<15 mV) over 300 cycles at 0.3 mA cm −2 . The Li−O 2 batteries assembled with the Li@Super P anode and LiI additive could mitigate the detrimental shuttling effect of I 3 − and deliver a high reversible capacity of 1000 mAh g −1 with a median charge voltage lower than 3.3 V after 50 cycles. This study provides a simple yet effective way to protect the lithium anode and design high-performance Li−O 2 batteries.

CAS / MDL: 10377-51-2
研究领域: 材料科学 · 电化学 · 电池技术
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Molecular Catalysis · 2023 · IF 4.6

Facet-dependent Pd0-O2−-Ce3+ active site for selective hydrogenation of linoleate ester to cis oleic acid ester

Minghao Zha,Hao Yan,Ruiying Li,Yinghao Sun,Ruitong Wang,Yibin Liu,Xiaobo Chen,Xin Zhou,Xiang Feng,Chaohe Yang

Reducing the formation of trans fatty acid in vegetable oil hydrogenation process is of significance to ensure food safety. Herein, Pd 0 -O 2− -Ce 3+ active site was constructed by strong electronic interactions between Pd 0 and CeO 2 -Polyhedrons to promote the formation of cis fatty acid. Results reveal that the abundant oxygen vacancies of CeO 2 (111) facets promote the adsorption and activation of hydrogen, leading to excellent catalytic activity of Pd/CeO 2 -Polyhedrons. Moreover, electronic reconstructed Pd 0 -O 2− -Ce 3+ active site limits the σ-bond rotation of half-hydrogenated intermediates through enhancing π backdonation and weakening the σ-bond, contributing to the reduction of trans products. Under mild conditions (30 °C, 0.3 MPa H 2 , and 2 h), Pd/CeO 2 -Polyhedrons catalyst shows exceptional methyl oleate selectivity of 52.6% with 93.8% conversion for sunflower oil hydrogenation. The catalyst has been further extended to the selective hydrogenation to several other vegetable oils such as sunflower oil, peanut oil, soybean oil, among others, under mild conditions.

研究领域: 催化化学 · 食品安全 · 材料科学
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POLYMER · 2024 · IF 4.1

Solvent-induced microphase separation membranes of block poly (aryl ether sulfone) copolymer with high selectivity of O2/N2 separation

Zhe Cheng,Pei Wang,Yunlong Sun,Zhipeng Wang,Guangyuan Zhou

Gas separation membranes have a wide range of applications in industry, and there are two important factors in judging membrane standards permeability and selectivity. How to improve the selectivity of gas separation membranes while improving permeability is a challenge. In this study, poly (aryl ether sulfone) (PES) block copolymers were synthesized from fluorine-terminated polysulfone (PSF–F) and hydroxyl-terminated cardo PES containing phenyl substituted isoindolinone side group (PES-PPI-OH). Large side groups can enlarge the free volume and hinder chain movement to improve gas permeation behavior. Solvent-induced microphase separation of block copolymers by casting membranes with solvent benzyl alcohol (BA) can improve selectivity. The PSF- b -PES-PPI (10:10) BA membrane maintain good mechanical properties and tensile strength up to 93 MPa which compared to random polymer membrane rises to 14 MPa. Gas permeation at 23 °C showed that the O 2 /N 2 selectivity of PSF- b -PES-PPI (5:15)BA membrane was 10.6, which was the 2008 Robeson upper bound. Thus, poly (aryl ether sulfone) materials showed great potential application for O 2 /N 2 separation.

CAS / MDL: 126-33-0
研究领域: 材料科学 · 化学工程
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Nanoscale · 2021 ·Vol. 13 ·期 16 ·7774-7782 · IF 7.79

Rational design of N-doped CNTs@C3N4 network for dual-capture of biocatalysts in enzymatic glucose/O2 biofuel cells

Gangyong Li,Guangming Ren,Wei (Alex) Wang,Zongqian Hu

Carbonaceous materials are promising electrode materials for enzymatic biofuel cells (EBFCs) due to their excellent electrical conductivity, chemical and physical stability and biocompatibility. Design and preparation of carbon materials with a hollow structure and a rough surface are of great significance for immobilization of enzymes both inside and outside the carbon materials for EBFC applications. We report herein the synthesis of novel carbonaceous materials consisting of bamboo-shaped hollow N-doped carbon nanotubes (N-CNTs) and C3N4 nanosheets (denoted as N-CNTs@C3N4) as electrode materials for dual-capture of enzymes in glucose/O2 EBFCs. The combination of one-dimensional N-CNTs with an open structure and two-dimensional C3N4 nanosheets forms a three-dimensional crosslinking network that significantly enhances the immobilization of enzymes, electrode stability, and mass transfer of substrates, thus boosting the EBFC performance. As a result, EBFCs equipped with N-CNTs@C3N4 can generate a high open circuit potential of 0.93 V and output a maximum power density of 0.57 mW cm−2 at 0.47 V. Additionally, the as-fabricated glucose/O2 EBFCs are capable of directly harvesting energy from various soft drinks, which indicates the promising applications of the N-CNTs@C3N4 nanocomposite as an electrode material for EBFCs.

研究领域: 材料科学 · 电化学 · 生物催化
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