CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Liyang Zhang,Yangqin Gao,Ziyu Teng,Yida Liu,Xinming Liu,Chuanbo Cong,Kezhen Lai,Linping Li,Jipeng Dong,Ning Li,Lei Ge
Mimicking the movement of leaves in response to external stimulations is inspiring for designing photocatalyst system applicable in space- and weight-sensitive scenarios. Here, we demonstrate that by combining a novel gas–liquid film growth process with a tape assisted film transfer procedure driven by capillary force, a lightweight and twistable photocatalyst assembly can be easily constructed. Taking the gas–liquid interface as a solute transfer boundary to selectively trigger the film growth at the interface, BiOI and BiOI/In 2 O 3 thin films up to 15 cm in diameter can be grown at a solution surface. Thanks to the capillary force present at the dynamic contact front during the film pick-up procedure, the grown film can be peeled off from the solution surface with tape so that a lightweight BiOI/In 2 O 3 /tape assembly can be easily constructed. Due to its low density and the BiOI/In 2 O 3 heterojunction formed, the resulting BiOI/In 2 O 3 /tape assembly exhibits superior photocatalytic activity per gram towards NO removal. Furthermore, the capillary force driven film pick-up process also induces a tight contact between the film and the tape, which makes the assembly highly twistable: its structural integrity and photocatalytic activity are largely preserved after 10,000 twists. Utilizing the film’s flexibility and twistability, we assemble a temperature-, auto-folding/unfolding photocatalyst system by transferring the film onto a memory-alloy-based structure, which mimics the movement of leaves in response to external stimulations and makes the gas–liquid interface-derived BiOI/In 2 O 3 /tape assembly suitable for use in space- and weight-limited environments.
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Journal of Materials Chemistry A
·
2024
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IF 10.7
Honghong Yi,Ruzhu Jia,Xiaolong Tang,Dongjuan Kang,Qingjun Yu,Fengyu Gao,Shunzheng Zhao,Yunpeng Liu
Electrocatalyst reduction of nitrogen oxides (NOx) in the industrial flue gas to synthesize NH3 can not only greatly improve the electrochemical efficiency of NH3 production, but also realize the emission reduction and resource utilization of air pollutants. Purposeful structural optimization of catalysts is a key research challenge in this field. Firstly, density functional theory (DFT) calculations found that the formation of surface oxygen vacancies could be promoted by constructing metal cation vacancies on the catalyst surface, which in turn optimized the NO adsorption configuration and improved the catalytic activity. By this guidance, CoAl layered double hydroxides (CoAl-LDH) nanosheets containing Al atomic vacancies were prepared by alkali etching. Experimental results show that a suitable alkali etching time with aqueous NaOH can significantly enhance the electrocatalytic activity of the CoAl-LDH nanosheets for NO reduction to NH3. Compared with pristine CoAl-LDH (0.097 mg cm-2 h-1), the NH3 yield rate reached 0.310 mg cm-2 h-1 at -1.1 V vs. the reversible hydrogen electrode after alkali etching for 4 h, which increased by 2.2 times. The catalyst characterization and theoretical calculation results indicate that the abundant frustrated Lewis pairs (FLPs) on the surface of catalysts containing cation vacancies are the origin of the enhanced activity.
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Bioactive Materials
·
2025
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IF 20.3
Haiyan Yao,Emine Sumeyra Turali Emre,Yuan Fan,Jiaolong Wang,Feng Liu,Junchao Wei
Periodontitis is a chronic inflammatory disease characterized by progressive alveolar bone resorption, and excessive reactive oxygen species (ROS) is a key factor to disease progression. Therefore, scavenging ROS to alleviate inflammation and promote bone regeneration are promising strategies to treat periodontitis. In this study, L-arginine (L-Arg) was used to modify mesoporous bioactive glass (MBG), forming L-Arg modified MBG (MBG@L-Arg), which showed effective ROS-scavenging and NO release properties in cells, and realize the protection and restoration of cell's activity in ROS-rich microenvironment. Furthermore, MBG@L-Arg can induce macrophage polarization from M1 to M2 phenotype, and promote the osteogenic differentiation of MC3T3-E1 cells and human periodontal ligament stem cells (hPDLSCs). MBG@L-Arg also regulated anti-inflammatory and antioxidant systems by inhibiting the NF- κ B signaling pathway and activating the Nrf2 signaling pathway. Besides, NO-PKG signaling pathway was also activated, further promoting bone regeneration. The in vivo results demonstrated that MBG@L-Arg can efficiently inhibit inflammation-induced tissue destruction and promote osteogenesis regeneration. The quantitative bone loss in MBG@L-Arg group was 1.03 ± 0.05 mm, significantly lower than that of the periodontitis group (1.47 ± 0.13 mm), implying that MBG@L-Arg can work as multifunctional materials for periodontal tissue regeneration.
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PubMed
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Tianjiao Wu,Bibo Ma,Huanhuan Bai,Lin Wang,Yumei Zhang,Qingzhi Luo,Jing An,Huiying Mu,Desong Wang,Yandong Duan
Developing highly efficient photocatalysts that selectively convert NO pollutants to NO 3 ¯ while storing metabolic nitrogen for crops remains a great challenge. Simultaneously, there is a dearth of research investigating the relationship between the chemical environment and the activity of catalytic sites. Herein, an efficient impregnation approach to access atomically dispersed Sr single atoms supported on Nb 2 O 5 is reported; meanwhile, various ligands (-Cl, -Br, -OH) are employed to customize the local structure. The results show that Cl-Sr/Nb 2 O 5 exhibits excellent catalytic performance in eliminating NO, which is significantly superior to other catalysts. The introduction of Sr atom and ligand increases the energy barrier of NO 2 formation, thus improving the selectivity of converting NO to NO 3 ¯. This study highlights the importance of precisely designing the catalytic site at the atomic level, and the obtained insights may serve as a valuable guide for developing future catalyst designs.
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Biomaterials Science
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2024
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IF 5.8
Xiaoli Tang,Yong Li,Tao Zhu,Longhao Lv,Jinliang Liu
X-ray-excited photodynamic therapy (X-PDT) employs X-rays as an energy source, overcoming the light penetration limitations of traditional photodynamic therapy (PDT) but is constrained by high-energy radiation and the hypoxic tumor microenvironment. Low-dose X-ray-excited photodynamic therapy and reduction of mitochondrial oxygen consumption can serve as significant breakthroughs in overcoming these barriers. In this study, NaLuF4:Tb/Gd (15%/5%)@NaYF4 (ScNP) nanoparticles adsorbing the photosensitizer MC540 and loaded with α-(nitrate ester) acid (NEAA) were prepared as low X-ray dose triggered nano-scintillators. The final product obtained was NaLuF4:Tb/Gd (15%/5%)@NaYF4@mSiO2@MC540@NEAA (ScNP-MS@MC540@NEAA) nanocomposites, which exhibited intense green luminescence. X-PDT generates cytotoxic reactive oxygen species (ROS) with minimal ionizing radiation damage. Simultaneously, NEAA reacts with glutathione (GSH) to generate nitric oxide (NO) for gaseous treatment of the damaged mitochondrial respiratory chain to reduce oxygen consumption and alleviate hypoxia, enhancing the X-PDT efficacy and realizing a closed-loop treatment. The superoxide ions (˙O2−) can rapidly react with NO produced to form the highly cytotoxic reactive nitrogen species (RNS) peroxynitrite anion (ONOO−), which exhibits higher cytotoxicity compared to ROS. Furthermore, GSH scavenges toxic ROS and maintains the physiological function of tumor cells. It can induce cancer cell overoxidation and nitrosative stress. This work describes a low-dose X-ray-triggered X-PDT system with total radiation of 50 mGy, which involves GSH consumption, self-supplied NO, mitochondrial damage alleviation, and hypoxia relief to generate ROS and RNS, forming a closed-loop anti-hypoxia dual-mode system with synergistically enhanced anti-tumor effects, without significant biological side effects. It provides a promising platform for deep-seated tumor X-PDT with considerable application prospects.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 9
·2452-2460
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IF 4.4
Xiao Tan,Suitao Qi,Guangxu Cheng,Chunhai Yi,Bolun Yang
As the ideal NO removal technology, the biggest challenge associated with the direct catalytic decomposition of NO is the development of highly active deNOx catalysts at low temperatures. Herein, a composite metal catalyst, Rh(0.2)/NC-MnFe, was prepared via impregnation for the low-temperature direct decomposition of NO, which exhibited 99.6% NO conversion and 63% N2 selectivity at 150 °C, and nearly 100% NO conversion and 98% N2 selectivity at 200 °C. The characterization results showed that the Rh(0.2)/NC-MnFe catalyst possessed a regular nanocage structure, good crystallinity, and suitable specific surface area. Its excellent low-temperature activity was attributed to the transfer of the dissociated O of NO from the Rh active site to the NC-MnFe support, which effectively inhibited the deactivation of Rh. The mechanism analysis indicated that NO adsorbed on the Rh(0.2)/NC-MnFe catalyst surface can generate NO2− and NO3−, and then the adsorbed NO together with NO3− is converted to NO2− species accompanied by the release of N2O. At last, NO2− is decomposed to N2.
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Bioactive Materials
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2025
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IF 20.3
Yuanyuan Peng,Wei Feng,Hui Huang,Yu Chen,Shaoling Yang
Senescent-endothelial cells significantly accelerate atherosclerosis progression, making the mitigation of cellular aging a promising strategy for treating the disease. Nitric oxide (NO), a low molecular weight and lipophilic gas, has been shown to penetrate cell membranes effectively and delay cell senescence. In this study, we designed and engineered osteopontin (OPN)-modified nanoliposomes (CZALO) that encapsulate L-arginine (L-Arg) and cerium-zirconium oxide nanoparticles (CZ NPs), which exhibit enzyme-like activities for targeted atherosclerosis treatment. Following inflammatory chemotaxis and OPN-mediated internalization by macrophages, CZ NPs released from CZALO nanoliposomes significantly scavenge reactive oxygen species, thereby inhibiting cholesterol uptake and promoting macrophage phenotypic transformation, resulting in both antioxidant and anti-inflammatory effects. Additionally, nitric oxide synthase (NOS) overexpressed in macrophages catalyzes L-Arg to produce NO, which is then selectively released in situ and diffuses into endothelial cells, exerting anti-aging effects by regulating senescence-associated secretory phenotype factor secretion, enhancing lysosomal function, alleviating cell cycle arrest, and reducing DNA damage. The antioxidant and anti-aging effects of CZALO nanoliposomes collectively alleviate atherosclerotic burden with minimal toxicity both in vitro and in vivo . This “two-birds-one-stone” nanotherapeutic offers a novel approach for regulating vascular microenvironment homeostasis and improving therapeutic efficiency in atherosclerosis treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Hao Ma,Chunyan Huang,Tianqi Tan,Wenting Li,Wei Xu,Yu Shen,Yuhan Li,Ruimei Fang,Fan Dong
Photocatalytic technology is of great significance in environmental purification due to its eco-friendly and cost-effective operations. However, low charge-transfer efficiency restricts the photocatalytic activity of the catalyst. Herein, we report Cs 2 SnBr 6 /C 3 N 4 composite catalysts that exhibit a robust interfacial electron exchange thereby enhancing photocatalytic nitric oxide (NO) oxidation . A comprehensive study has demonstrated the S-scheme electron transfer mechanism. Benefiting from the interfacial internal electric field , the C-Br bond serves as a direct electron transfer channel, resulting in enhanced charge separation. Furthermore, the S-scheme heterojunction effectively traps high redox potential electrons and holes, leading to the production of abundant reactive oxygen radicals that enhance photocatalytic NO abatement. The NO removal rate of the Cs 2 SnBr 6 /C 3 N 4 heterogeneous system can reach 86.8 %, which is approximately 3-fold and 18-fold that of pristine C 3 N 4 and Cs 2 SnBr 6 , respectively. The comprehensive understanding of the electron transfer between heterojunction atomic interfaces will provide a novel perspective on efficient environmental photocatalysis .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zanyun Ying,Xinya Wang,Chengzhi Wu,Shihan Zhang
Photocatalytic NO degradation often suffers from sluggish charge carrier separation and low selectivity. Herein, a series of In 2 O 3 /TiO 2 (P25) composites were synthesized to enhance NO abatement. Benefiting from the conspicuous synergistic effect between In 2 O 3 and P25, the In 2 O 3 /P25 catalysts demonstrated more than double the NO elimination performance compared to pure P25 and In 2 O 3 . The In 2 O 3 /P25 sample with 75 wt% In 2 O 3 (In-P25-75) achieved a NO removal efficiency of 51.7 %, higher than reported catalysts (30.0–49.0 %). It was the successful formation of type-II heterostructure that enabled intimate interfacial contact and provided ample electron transfer channels. Moreover, photoluminescence spectra and photoelectrochemical measurement confirmed the improved separation and inhibited recombination of photogenerated charge carriers in In-P25-75, thereby boosting the NO photocatalytic efficiency. ·O 2 − and ·OH radicals generated by photoinduced electron transfer to the conduction band of P25, along with the induced holes confined to the valence band of In 2 O 3 , facilitated the targeted deep oxidation of trace NO into NO 3 − rather than harmful NO 2 . This work discloses a promising strategy for the efficient removal of NO from the atmosphere by reducing the emission of hazardous intermediate NO 2 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yinglin Liang,Kui Yang,Xinfei Zhang,Weiting He,Xiangtong Kong,Yang Zhou,Jinxing Ma
The formation of chlorinated by-products in the treatment of chloride-laden water/wastewater by advanced oxidation processes (AOPs) has become a severe challenge to their environmentally benign application. Herein, we propose an efficient and safe alternative, i.e. , flow-through anodic oxidation (FTAO) system based on the nonradical direct electron transfer (DET) process at low voltage. By controlling the anode potential below the threshold for chlorine evolution at the anode, this system achieved zero formation of inorganic and organic chlorinated byproducts whilst significantly eliminated the biotoxicity of the parent micropollutant. Meanwhile, due to the nonradical direct oxidation mechanism, the voltage-confined FTAO system attained high efficiency and selectivity for the micropollutant removal from a complex matrix containing naturally co-existing anions and organic matter. The feasibility of FTAO applications was further evaluated by removing various pollutants (including antibiotics and phenols) from actual municipal effluent and surface water. More than 96% percentage removal was achieved at extremely low energy consumption (0.003–0.017 kWh m −3 ). In summary, our results provide insight into the development of novel electrochemical technologies free from secondary pollution towards environmental remediation applications and beyond.
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Nature Catalysis
·
2023
·Vol. 6
·期 10
·906-915
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IF 37.8
Li Mengyang,Wu Yongmeng,Zhao Bo-Hang,Cheng Chuanqi,Zhao Jinghui,Liu Cuibo,Zhang Bin
Amino acids have wide application in the food and pharmaceutical industries. Current biotic and chemical syntheses suffer from low efficiency, complex purification operations and high energy consumption. Here we report a sustainable electrocatalytic synthesis of alanine from NO and pyruvic acid over oxide-derived Ag with low-coordination sites under ambient conditions. Mechanistic studies reveal a cascade NO → NH 2 OH → pyruvate oxime → alanine pathway. The quick pyruvate oxime formation and slow pyruvate oxime reduction steps cause various side reactions, leading to low alanine production. Then, a spatially decoupled two-pot electrosynthesis system using flow reactors loaded with oxide-derived Ag is designed for pyruvate oxime formation and reduction reactions. This decoupled system delivers 3.85 g of easily purified alanine with a total Faradaic efficiency of 70% and a purity of >98% at 100 mA cm −2 . Further techno-economic analysis demonstrates the potential. This method is suitable for solar-energy-driven alanine electrosynthesis from polylactic acid wastes and for the fabrication of other amino acids.
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Heliyon
·
2024
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IF 3.4
Yige Guo,Xiaoxue Niu,Huaiyu Yang,Liwen Chen,Yizhen Ren,Huining Guo,Bo Wu
The oxidation rate of NO to NO 2 is a critical parameter in the removal of NO x within selective catalytic reduction (SCR) systems. LaCoO 3-δ is a kind of potential catalyst to enhance the oxidation of NO to NO 2 , it may offers an economic and stable alternative to noble metal catalysts, particularly at elevated temperatures. This study aimed to enhance the catalytic efficiency of LaCoO 3-δ through strontium (Sr) doping. La 1-x Sr x CoO 3-δ (with varying x values of 0.1, 0.2, 0.3, 0.4) was synthesized using a sol-gel method. La 1-x Sr x CoO 3-δ exhibited superior NO oxidation catalytic activity compared to LaCoO 3-δ , with the most notable enhancement observed at x = 0.3 (84 % conversion). This improvement can be attributed to the substitution of La 3+ with Sr 2+ , which induces lattice distortion and charge imbalance, thereby creating more oxygen vacancies that enhance the catalytic oxidation capability of La 1-x Sr x CoO 3-δ . However, it's important to note that an excessive amount of Sr can result in the formation of SrCO 3 deposits on the surface of La 1-x Sr x CoO 3-δ , thereby diminishing its catalytic oxidation performance. The catalytic oxidation reaction behavior adhered most closely to the O 2 -adsorbed E-R model, the surface defects in La 1-x Sr x CoO 3-δ playing a pivotal role in the catalytic reaction.
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