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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Tubular g-C3N4 coupled with lanthanide oxides Yb2O3 as a novel bifunctional photocatalyst:Enhanced photocatalytic NO removal and H2 evolution, dual regulation and reaction pathway

Youzhou He,Mingzuo Chen,Yao Jiang,Lei Tang,Jianning Yu,Ya Chen,Min Fu,Xuemei Tan,Jiajia Jing,Guizhi Zhang,Xingyan Liu

The modification of graphite carbonitride (g-C 3 N 4 ) is beneficial to increase its specific surface area and high quantum efficiency, thus improving its activity. Herein, the Yb 2 O 3 /g-C 3 N 4 composites were adjusted through dual regulation synergistically (nanostructure design of g-C 3 N 4 and addition of lanthanide oxides Yb 2 O 3 ) to improve the photocatalytic performance of hydrogen production and NO removal simultaneously. The as-prepared 1% Yb 2 O 3 /tubular g-C 3 N 4 could efficiently promote the photocatalytic hydrogen evolution (4071.763 μmol·g −1 ·h −1 ) and NO removal performance (54.20%), which was approximately 8.85 times and 32.01% higher respectively than that of bulk g-C 3 N 4 prepared by melamine (g-C 3 N 4 -M). The formation process of·O 2 - and·OH radicals and the oxidation process of NO had been systematically studied through ESR and in-situ DRIFTS , which proved that the coupling of tubular g-C 3 N 4 with Yb 2 O 3 had a positive effect. This work provided a novel strategy for dual regulation (adjust morphology and metal oxide introduction) synergistically design of bifunctional photocatalysts to enhance H 2 production and NO removal simultaneously.

CAS / MDL: 35725-34-9
研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Oxygen vacancy defects-boosted deep oxidation of NO by β-Bi2O3/CeO2-δ p-n heterojunction photocatalyst in situ synthesized from Bi/Ce(CO3)(OH) precursor

Junli Nie,Gangqiang Zhu,Weibin Zhang,Jianzhi Gao,Peng Zhong,Xiaotao Xie,Yu Huang,Mirabbos Hojamberdiev

Flower-like n -type CeO 2-δ is hybridized with p -type β-Bi 2 O 3 nanoparticles to design a novel β-Bi 2 O 3 /CeO 2-δ p - n heterojunction photocatalyst via a thermal treatment process of Bi/Ce(CO 3 )(OH) precursor. The synthesized β-Bi 2 O 3 /CeO 2-δ exhibits a remarkable enhancement in NO removal and significant suppression of toxic intermediates nitrogen dioxide (NO 2 ) under visible light irradiation. The superior photocatalytic activity of β-Bi 2 O 3 /CeO 2-δ for NO removal is mainly derived from the synergistic effects of the oxygen vacancies (OVs) and p-n heterojunction. The OVs not only enhance the visible light utilization and boost the separation of electron-hole pairs but also improve the adsorption and activation of NO and O 2 . Particularly, the p-n heterojunction is beneficial for the interfacial migration of photogenerated charge carriers. Electron spin resonance (ESR) and trapping experiment reveal that the synergistic effects of OVs and p-n heterojunction can induce the generation of more active species. The electrochemical measurements and density-functional theory (DFT) calculations in-depth confirm that both p-n heterojunction and OVs can accelerate the interfacial charge transfer, resulting in the deep oxidation of reactants. Therefore, the flower-like β-Bi 2 O 3 /CeO 2-δ p-n heterojunction photocatalyst exhibits an advanced photocatalytic activity for deep NO removal and a suppressed NO 2 generation. In addition, monitoring the reaction products by in situ Fourier transform infrared spectrum (FTIR) further validates that the main products of nitrates are formed during the photocatalytic process. This work demonstrates a straightforward approach for construction of p-n heterojunction photocatalysts, which can enhance the effective photocatalytic activity and stability for NO removal.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2019 · IF 6.361

Boosting the low-temperature activity and sulfur tolerance of CeZr2Ox catalysts by antimony addition for the selective catalytic reduction of NO with ammonia

Xiaoqiang Wang,Yue Liu,Weiyuan Yao,Zhongbiao Wu

In this paper, a series of Sb modified CeZr 2 O x mixed oxides (Sb y CZ) were synthesized by citrate method for the selective catalytic reduction of NO with ammonia (NH 3 -SCR). Experimental results exhibited that the Sb addition could bring a great improvement of SCR activity at 200–360 °C owing to the enhancement in surface area , redox ability and surface acidity . More importantly, the sulfur tolerance of the catalyst with proper Sb loading contents was dramatically improved. For instance, above 85% deNO x efficiency was retained over Sb 0.5 CZ catalyst after 24 h reaction in the presence of 100 ppm SO 2 and 5 vol.% H 2 O. As for pure CeZr 2 O x and the catalysts with low Sb loading contents, the serious accumulation of ammonium sulfates resulted in the deactivation after SO 2 exposure. However, with excessive Sb addition, more labile oxygen readily reacted with SO 2 and the redox cycle was then disrupted, leading to the decrease of SCR activity. With an appropriate Sb loading contents, the sulfate species preferentially formed around Sb cations could restrain the further consumption of oxygen species in Ce-O-Ce or Ce-O-Zr mode by SO 2 via a space confinement effect. Thus, a certain amount of labile oxygen was preserved to drive the SCR reaction, thereby enhancing the sulfur tolerance of the catalyst.

研究领域: 催化 · 环境化学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Designing multivariate porphyrin-based metal-organic frameworks with Ni/Co dual-metal atom sites for cooperative NO2 capture and NO retention

Shanshan Shang,Chao Yang,Yuanmeng Tian,Zeyu Tao,Mallory Smith,Hongyan Zhang,Lin Zhang,Liangchun Li,Qinfen Gu,Hong-Cai Zhou,Yong Sik Ok,Jin Shang

Selective adsorption using porous materials is a promising approach to removing ambient nitrogen dioxide (NO 2 ). However, the highly reactive nature of NO 2 and the often-associated release of nitric oxide (NO) render a formidable challenge in developing effective and stable adsorbents. Here, we designed multivariate porphyrin-based metal–organic frameworks (MTV-PMOFs Al-PMOF(Ni x Co y )) featuring atomically dispersed Ni/Co dual-metal centers in the porphyrin ring as active adsorption sites, as robust adsorbents capable of synergistically boosting NO 2 adsorption capability and retaining the evolved NO. The introduction of the Ni/Co dual-metal sites in MTV-PMOFs greatly enhanced the NO x adsorption performance. Under dry conditions, Al-PMOF(Ni 1 Co 1 ) exhibited a NO 2 adsorption capacity of 3.66 mmol/g (100 ppm NO 2 in feed), among the highest under similar conditions, a high NO retention ability, and good regenrability (85%). Under wet conditions, its NO 2 removal capacity was further elevated by more than 50% (5.65 mmol/g). Moreover, the Ni/Co ratio in MTV-PMOFs dictates a structure–property relationship between the released amount of NO and adsorbed capacity of NO 2 . Such a corporative NO 2 and NO adsorption was for the first time established in MOFs. The material stability and potential economic value were also investigated to demonstrate the applicability of MTV-PMOFs as NO 2 adsorbents. This work provides new perspectives for the development of adsorption-based technology for mitigating ambient NO 2 pollution and managing other corrosive and toxic gases.

CAS / MDL: 6147-53-1 6018-89-9
研究领域: 材料科学 · 环境科学
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Catalysts · 2018 ·Vol. 8 ·期 12 ·642 · IF 3.465

Structure–Activity Relationship Study of Mn/Fe Ratio Effects on Mn−Fe−Ce−Ox/γ-Al2O3 Nanocatalyst for NO Oxidation and Fast SCR Reaction

Yan Gao,Tao Luan,Mingyang Zhang,Wenke Zhang,Wenchen Feng

A series of Mn−Fe−Ce−Ox/γ-Al2O3nanocatalysts were synthesized with different Mn/Fe ratios for the catalytic oxidation of NO into NO2and the catalytic elimination of NOxvia fast selective catalytic reduction (SCR) reaction. The effects of Mn/Fe ratio on the physicochemical properties of the samples were analyzed by means of various techniques including N2adsorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature-programmed reduction (TPR), NH3-temperature-programmed desorption (TPD) and NO-TPD, meanwhile, their catalytic performance was also evaluated and compared. Multiple characterizations revealed that the catalytic performance was highly dependent on the phase composition. The Mn15Fe15−Ce/Al sample with the Mn/Fe molar ratio of 1.0 presented the optimal structure characteristic among all tested samples, with the largest surface area, increased active components distributions, the reduced crystallinity and diminished particle sizes. In the meantime, the ratios of Mn4+/Mnn+, Fe2+/Fen+and Ce3+/Cen+in Mn15Fe15−Ce/Al samples were improved, which could enhance the redox capacity and increase the quantity of chemisorbed oxygen and oxygen vacancy, thus facilitating NO oxidation into NO2and eventually promoting the fast SCR reaction. In accord with the structure results, the Mn15Fe15−Ce/Al sample exhibited the highest NO oxidation rate of 64.2% at 350 °C and the broadest temperature window of 75–350 °C with the NOxconversion >90%. Based on the structure–activity relationship discussion, the catalytic mechanism over the Mn−Fe−Ce ternary components supported byγ-Al2O3were proposed. Overall, it was believed that the optimization of Mn/Fe ratio in Mn−Fe−Ce/Al nanocatalyst was an extremely effective method to improve the structure–activity relationships for NO pre-oxidation and the fast SCR reaction.

研究领域: 环境科学 · 催化化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Fabrication of SiC catalytic filter with low vanadium loading and highly uniform structure for efficient NO reduction and dust removal

Xiangsen Xu,Jiangxiao Qiao,Shibo Yu,Jiahao Chen,Yiqing Zeng,Feng Zhang,Zhaoxiang Zhong,Weihong Xing

The rational design of catalysts and the establishment of uniform filter structure are key points in the development of high-performance catalytic filters. To resolve the issue of increased N 2 O concentration in catalysts with high vanadium content at high temperatures, a range of catalytic filters with low vanadium loading were fabricated by partially substituting vanadium in 6VWTi catalysts with transition metals (Mn, Cu, Co and Ce). The experimental results show that the introduction of Ce, which leads to rich surface-adsorbed reactive oxygen species, good redox properties and appropriate surface acidity, thus the 1V5CeWTi/SiC catalytic filter exhibits the highest denitration efficiency (NO conversion >90 % at the temperature of 300–500 °C without N 2 O production), presenting significant advantages in contrast to 1VWTi/SiC and 6VWTi/SiC. Furthermore, the preparation technology was optimized to obtain a more uniform structure, which enhanced NH 3 -SCR performance and reduced filter pressure drop. The optimized 1V5CeWTi/SiC also exhibited exceptional resistance to SO 2  + H 2 O and long-term stability for a duration of 200 h at 300 °C, as well as displays a noteworthy efficiency in filtering particulate matter (10 μm SiO 2 ). Therefore, the optimized 1V5CeWTi/SiC catalytic filter holds great potential in the realm of gas purification.

研究领域: 环境工程 · 催化 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

A superior Fe-Zr mixed oxide catalyst for the simultaneous reduction of NO and SO2 with CO

Liam John France,Wan Li,Yanke Zhang,Wentao Mu,Zhihang Chen,Junjun Shi,Qiang Zeng,Xuehui Li

A series of Fe-Zr mixed-metal oxides were prepared and examined for the simultaneous reduction of NO and SO 2 with CO. The catalyst containing 40 mol% exhibited near-complete conversion of both pollutants at a minimum temperature of 350 °C and a GHSV of 90,000 h −1 . The addition of Fe 3+ to ZrO 2 decreased the crystallinity of the latter phase and significantly enhanced surface area. Concentrations of 30 mol% or greater produced segregated FeO x phases, which affected catalytic performance in distinctly different ways: supported Fe 3+ (30 mol%) possessed similar activity to doped Fe 3+ ; α-Fe 2 O 3 (50 mol%) inhibited activity due to its’ lower reducibility; an amorphous phase (40 mol%) promoted iron-weighted areal activity. A complete identification of the ambiguous component was not successfully established, but the obtained properties revealed that it exhibited weaker interaction with the support and had a size greater than that of oligomeric-Fe 2 O 3 yet smaller than 3 nm.

CAS / MDL: 77-92-9 5949-29-1
研究领域: 催化 · 环境科学 · 化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Photothermal effect induced humidity-resistant photocatalytic NO removal over dual-defects modified Bi/Bi4Ti3O12

Xue Xiao,Qiuhui Zhu,Jiapeng Hu,Yin Shen,Yu Huang,Yuanhao Wang,Chuanyi Wang

Photocatalysis is appealing in removing trace NO, but its efficacy is often deteriorated by H 2 O, which is ubiquitous in environment, and how to resolve this issue and elucidate the underlying mechanisms at the molecular-level are challenging. Herein, we report a full-spectrum Bi/Bi 4 Ti 3 O 12 catalyst modified with Bi-O vacancy associates via a steam-assisted chemical reduction process. The optimized structure demonstrates NO removal efficiency of 75.5 %, four times over its counterpart, Bi 4 Ti 3 O 12 (37.9 %). Based on positron annihilation spectra and theoretical studies, the enhanced activity is induced by Bi-O vacancy associates, which not only optimizes the photogenerated carrier dynamical behaviors but lowers the energy barriers for photocatalytic oxidation of NO. Importantly, the photothermal activity of the optimal sample exhibited a decline from 76.7 % (0 % RH) to 71.2 % (100 % RH), whereas its photoactivity (20°C) demonstrated a more pronounced decrease, dropping from 60.1 % (0 % RH) to 41.2 % (100 % RH). Therefore, humidity-resistant performance over the optimal sample is attributed to photothermal effect induced by in-situ precipitated Bi and multiple defects. Furthermore, the results of adsorption and desorption behavior of H 2 O and in situ DRIFTS suggest the photothermal-assisted desorption of surface-bound H 2 O can suppress the interactions of H 2 O and stable bidentate nitrate ( bi -NO 3 ⁻) by hydrogen bonds to generate monodentate nitrate ( m -NO 3 ⁻), thereby hindering the photodecomposition of m -NO 3 ⁻ to NO/NO 2 . This work elucidates the significance of photothermal effect in developing efficient photocatalyst for atmospheric NO purification in humid conditions.

研究领域: 环境催化 · 材料科学 · 大气污染控制 · 物理化学 · 纳米技术
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-14 · IF 16.6

Exploiting synergistic effect of CO/NO gases for soft tissue transplantation using a hydrogel patch

Tang Xiaoduo,Ren Jingyan,Wei Xin,Wang Tao,Li Haiqiu,Sun Yihan,Liu Yang,Chi Mingli,Zhu Shoujun,Lu Laijin,Zhang Junhu,Yang Bai

Autologous skin flap transplantation is a common method for repairing complex soft tissue defects caused by cancer, trauma, and congenital malformations. Limited blood supply range and post-transplantation ischemia-reperfusion injury can lead to distal necrosis of the flap and long-term functional loss, which severely restricts the decision-making regarding the optimal surgical plan. To address this issue, we develop a hydrogel patch that releases carbon monoxide and nitric oxide gases on demand, to afford a timely blood supply for skin flap transplantation during surgery. Using an ischemia-reperfusion dorsal skin flap model in rats, we show that the hydrogel patch maintains the immediate opening of blood flow channels in transplanted tissue and effective blood perfusion throughout the perioperative period, activating perfusion of the hemodynamic donor site. We demonstrate that the hydrogel patch promotes distal vascularization and long-term functional reconstruction of transplanted tissues by inhibiting inflammatory damage and accelerating blood vessel formation.

研究领域: 生物医学工程 · 组织工程 · 再生医学 · 外科技术 · 药学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Glucose-responsive multifunctional hydrogel incorporating GOx@ZIF-8 for NO/Zn2+-mediated antibacterial and pro-angiogenic diabetic wound healing

Jialiang Pan,Chenhong Liu,Zhiqiang Wang,Wenbo Shi,Tianhao Zhao,Qingcong Wei,Qing Zhang,Zhengyu Bai

The hyperglycemic microenvironment of diabetic chronic wounds is a major driver of severe bacterial infections, excessive inflammatory responses, and impaired angiogenesis, all of which delay wound healing. To address these challenges, we prepared a glucose oxidase (GOx)–loaded zeolitic imidazolate framework-8 (GOx@ZIF-8). Furthermore, a multifunctional hydrogel (AACZ) was fabricated by incorporating 5-methylfurfural– and L-arginine–grafted alginate and maleimide–grafted chondroitin sulfate with GOx@ZIF-8 through the Diels–Alder reaction. Results showed that immobilized GOx remained active for a longer time than of free GOx. At the wound site, GOx catalyzed the conversion of excess glucose to gluconic acid and hydrogen peroxide (H 2 O 2 ). The reduced pH in the local region induced Zn 2+ release from zeolitic imidazolate framework-8, simultaneously, H 2 O 2 mediated the generation of nitric oxide (NO) from L-arginine. The synergy between Zn 2+ and NO endowed AACZ with excellent antibacterial properties. The biocompatible hydrogel promoted cell proliferation and migration, regulated local blood glucose levels, inhibited bacterial activity, alleviated inflammation and promoted angiogenesis and collagen deposition at the diabetic wound site. These findings suggest that AACZ holds promise as a responsive dressing material in healing for complex wounds.

研究领域: 生物材料 · 纳米医学 · 伤口愈合 · 生物化学 · 糖尿病研究
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Biofilm Microenvironment-Sensitive Piezoelectric Nanomotors for Enhanced Penetration and ROS/NO Synergistic Bacterial Elimination

Ye Zhao,Yao Liu,Ran Liao,Pan Ran,Yuan Liu,Zixuan Li,Jichun Shao,Long Zhao

Sonodynamic therapy offers a highly accurate treatment for bacterial infections; however, its antibacterial efficacy is hindered by bacterial biofilms that limit the penetration of sonosensitizers. Herein, a nitric oxide (NO)-driven mushroom-like Janus nanomotor (BT@PDA-La) based on the unilateral coating of polydopamine (PDA) on piezoelectric tetragonal barium titanate (BT) and further modified with l-arginine (l-Arg) on the PDA side is fabricated. In the infected microenvironment with high levels of H2O2, NO is produced unilaterally from BT@PDA-La, thus leading to its self-propelled movement and facilitating its permeability in the biofilm. Under ultrasonic vibrations, the piezoelectric effect of BT@PDA-La is triggered by the exogenous mechanical wave, and toxic reactive oxygen species (ROS) are efficiently generated via an in situ catalytic reaction. The synergistic treatment with ROS/NO achieved the destruction of biofilms and embedded drug-resistant bacteria in vitro. Importantly, BT@PDA-La exhibits excellent biofilm penetration capacity, effectively eliminating biofilm infection while accelerating the healing of infected muscles by alleviating oxidative stress, regulating inflammatory factors, and accelerating angiogenesis. Collectively, this study provides a promising strategy for enhancing the penetration of pathological environment-driven nanomaterials through biofilms and advances the application of nanomotors for the therapy of bacterial infections in clinical medicine.

研究领域: 纳米技术 · 生物医学工程 · 微生物学 · 治疗药物开发
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Surfaces and Interfaces · 2024 · IF 5.7

Effects of organic ligands and photoactive substances on MOFs-derived Co3O4@MnOx hollow-sphere structure for efficient energy transfer and photothermocatalysis of acetone and NO

Yanping Zhang,Yinian Zhu,Yinming Fan,Shengpeng Mo,Xiaobin Zhou,Zongqiang Zhu

A set of MOFs-derived Co 3 O 4 @MnO x hollow-sphere were synthesized to develop a catalyst for the photothermal catalytic removal of NO using acetone as a reducing agent. The study systematically investigated the impact of organic ligands and photoactive substances on energy transfer and photothermocatalytic reactions involving acetone and NO under 5 vol % H 2 O with the catalysts. At 240°C, sample C-5/1 (with an organic ligand added and Co/Mn molar ratio of 5/1) demonstrated 75 % NO conversion and 65 % acetone conversion. The highest catalytic performance was observed in the L-Py sample (with photoactive substance was added), achieving 80 % NO and 69 % acetone conversion at 240°C. The catalyst demonstrated low crystallinity, and the introduction structural defects through ligands adjusted the ratio of active components. Meanwhile, enhanced catalytic performance was attributed to light energy scattering in the inner space of microspheres, resulting in the efficient transfer of 2.17 eV energy with the addition of two photoactive substances. The elevated concentration of surface-active oxygen facilitated oxidation, while M n /M n+1 (Mn 3+ /Mn 4+ and Co 2+ /Co 3+ ) redox cycling supplied surface oxygen in the photothermal low-temperature response. The proposed mechanism for the simultaneous degradation of acetone and NO was elucidated using Density Functional Theory calculations.

研究领域: 环境科学 · 材料科学 · 催化化学
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