ACS Applied Nano Materials
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2024
·
IF 5.3
Wenying Zuo,Xiongdiao Lan,Guoyang Lv,Cuicui Yang,Ping Lan,Bo Peng,Pengru Liu,Ke Li
The oxygen evolution reaction (OER) is crucial for producing hydrogen through electrochemical water splitting using renewable energy sources. To enhance hydrogen production efficiency, an electrocatalyst with high efficiency and stability for OER is necessary. Layered double hydroxides (LDHs) are among the most active electrocatalysts for alkaline OER, but LDHs suffer from poor conductivity, potential agglomeration, and low intrinsic activity. Herein, sulfur–phosphorus codoping of CoFeLDH/MXene (S,P-CoFeLDH/MXene) nanoarray hybrid electrocatalyst was developed using a stripped Ti3C2Tx MXene substrate through an in situ growth strategy and sulfur–phosphorus codoping. The S,P-CoFeLDH/MXene electrocatalyst demonstrated remarkable activity and stability against oxygen evolution in alkaline media, with a low overpotential of 305 mV at 10 mA cm–2 and a Tafel slope of 39 mV dec–1. Moreover, the overpotential decreased by only 1.3% after 2000 CV cycles, surpassing the noble metal RuO2 catalyst. This effective strategy introduces an idea for a hybrid electrocatalyst designed for oxygen evolution, and the direct preparation method lays the groundwork for its broad application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Yunping Wu,Shuwen Niu,Zhengyu Wei,Lingzhe Meng,Wei Wei
Single-atom catalysts (SACs) with nitrogen-coordinated transition metal sites (M-N x ) hold great promise for electrocatalytic oxygen reduction and oxygen evolution reactions (ORR, OER). Despite substantial achievements based on the confinement pyrolysis and heteroatom-doping methods, the M-N x SACs still suffer from low yield of atomic sites and less tenability of electronic states of M-N x center. Here, an innovate synthesis methodology is proposed for surface integrating Co atoms onto polyoxometalate (POM) and its derivative clusters, which promise to regulate the atomic distribution and coordination environments of Co-N x SACs at the sub-nanometer level. The synthetic procedures exhibit general applicability for a variety of POM clusters to achieve high atomic Co loading up to 9.9 wt%. Steric integration by POM-derived clusters (e.g. MoN) also impart strengthened d-p orbital hybridization of Co-N x SACs by the formation of Co-N-Mo bonding, which surpass common heteroatoms toward modulating the geometric and electronic structures of M-N x SACs, leading to pronounced catalytic activity and durability. This work validates the effectiveness of the unique POM-integration strategy toward atomic dispersion of transition metal, further guides the engineering of M-N x SACs to promote catalytic performance from the sub-nanometer scale.
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POLYHEDRON
·
2025
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IF 2.6
Qian Du,Chang-Sheng Wang,Yu-Guo Yang,Wei Zhao,Xiao-Na Shen,Bing Liu,Yuan-Yuan Zhang,Hua-Di Zhang,Hua-Jian Yu,Cheng-Cheng Qiu,Xian-Shun Lv,Rui Zhang,Xu-Ping Wang
Some Tb 3+ /Eu 3+ doped SrGdGa 3 O 7 (SGGO) phosphors were fabricated, achieving multi-color tunability through the addition of a sensitizer. The experimental results indicate that the doped ions are uniformly distributed, with no impurity phases detected. In SGGO-based phosphors, Eu 3+ ions serve as activators and exhibit an optimal luminescence transition level of 5 D 0 → 7 F 4 . When Tb 3+ ions are used as the sensitizer and at a specific concentration, the luminescence color transition of green → orange → red as the content of Eu 3+ enhances. Analysis of the decay lifetime curves reveals that Tb 3+ → Eu 3+ energy transfers occur in the co-doped SGGO phosphors, with the mechanism identified as quadrupole–quadrupole interaction. This article investigates the specific energy transfer processes involved. The optimum content of Eu 3+ is ascertained as 0.03. Under the excitation at 375 nm, the SGGO based phosphor containing 0.06 Tb 3+ and 0.03 Eu 3+ exhibits CIE coordinates of (0.5000, 0.4397).
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Xuan Liu,Jie Chao,Feifei Guo,Liangliang Chang,Zengzhe Xi
To address rapid carrier recombination and low magnetic separation efficiency in piezocatalysis, Gd/Ni co-doped BiFeO3 nanoparticles were synthesized via a sol–gel method. Rietveld refinement confirmed lattice distortion and secondary phase formation at high doping levels. Gd/Ni doping induces a phase transition in BFO from rhombohedral to orthorhombic, with the Pnma proportion reaching 84.15% at x = 0.09. Gd/Ni co-doping induced 12.7% oxygen vacancy concentration, suppressing electron–hole recombination, while enhanced Dzyaloshinskii–Moriya interaction increased saturation magnetization by 17.85-fold (magnetic recovery > 95%). The optimized sample (x = 0.09) achieved 80.94% ofloxacin degradation in 120 min (twice that of pristine BiFeO3), retaining 71.53% efficiency after 4 cycles. Radical trapping and EPR identified ˙OH and ˙O2− as dominant species, revealing a ferroelectric–piezoelectric synergistic mechanism. This work provides a strategy for designing magnetically recoverable piezocatalysts for complex wastewater treatment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yi-Hong Yu,Xin Cui,Yi-Meng Hong,Gao-Wu Qin,Song Li
Incorporating electrochemical CO 2 reduction (ECR) that produces CO-rich syngas into the workflow of steelmaking presents a promising strategy to neutralize the steelmaking industry. Herein, we develop a highly efficient and stable Ag nanowires with surface CeO 2 armors (CeO 2 /AgNWs) as ECR electrocatalyst for syngas production. The engineered CeO 2 -Ag interface facilitates CO 2 -to-CO conversion by lowering the energy barrier for *COOH intermediate formation through synergistic electronic effects. At an industrially relevant current density of −251.3 mA cm −2 , the CeO 2 /AgNWs generate CO-rich syngas by co-electrolysis of CO 2 and H 2 O, with a high Faradaic efficiency (FE) of 92.1 % for CO. Techno-economic analysis (TEA) reveals that integrating the CeO 2 /AgNWs-driven ECR into existing steelmaking workflows can potentially reduce CO 2 emissions by 83 % and elevate the renewable energy utilization to ∼91.4 %, unlocking new possibilities for achieving carbon neutrality in the steel industry.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Ming Zhu,Daqin Guan,Zhiwei Hu,Hong-Ji Lin,Chien-Te Chen,Hwo-Shuenn Sheu,Shaobin Wang,Jing Zhou,Wei Zhou,Zongping Shao
Synergistic effects are often used in catalyst design for many environmental/energy applications, however, the mechanism and a molecular-level structure to exert maximal synergy effects in catalyzing advanced oxidation processes (AOPs) in wastewater remediation are still unknown. Here, by designing a model perovskite family R BaCo 2 O 6- δ ( R = lanthanides) with Co 4+ in octahedral coordination (Co4+ oct) and Co 3+ in pyramidal coordination (Co3+ pyr), we ambitiously confirm the unique synergy of unsaturated (Co3+ pyr) and metallic (Co4+ oct) Co sites for efficient peroxymonosulfate (PMS) activation. Combined X-ray adsorption spectra and theoretical calculations strongly demonstrate that Co3+ pyr and Co4+ oct synergistically contribute to PMS adsorption and O O bond cleavage, and facilitate Co 3+ /Co 4+ redox cycle for radical generation. With appropriate ratio and ordered distribution of Co3+ pyr/Co4+ oct, the Gd 0.5 La 0.5 BaCo 2 O 5.75 exhibits remarkable catalytic activity for pollutant degradation, outperforming all previously reported Co 4+ -related oxides. This work may inspire rational design of efficient metal oxide catalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Huajie Zhong,Junhui Wang,Bin Zhang,Yangyang Liu,Zeyu Gong,Xinzhe Xiao,Jiaxing Yu,Yu Hou,Yuan Tao,Huangsheng Yang,Qi Fu,Jiating Zheng,Pengfei Wang,Gangfeng Ouyang
Carbon-supported single-atom catalysts (CS-SACs) have attracted tremendous attention in environmental remediation fields, however, the role of the ubiquitously existing carbon defects on the support in regulating the electronic structure of active metal sites has long been overlooked. Herein, a selective pyridinic N etching strategy is proposed to controllably fabricate specific pentagon defects in the carbon supports anchored with Co-N 4 sites. Theoretical and experimental results reveal that the pentagon defects can induce upward shifting of the Co d-band center and increase the electron density in the dxz and dz 2 orbitals, indicating its indispensable role in regulating the electronic structure of the metal center. As a result, efficient electron transfer is realized between the Co atom and peroxymonsulfate (PMS). Moreover, the energy barriers for crucial oxygen intermediate are reduced, which facilitates the generation of singlet oxygen ( 1 O 2 ). Consequently, the Co-N 4 catalyst with pentagon defects (C5-Co-N 4 ) achieved a remarkable TOF value (9.37 min −1 ) in a Fenton-like reaction, surpassing the state-of-the-art single-atom catalysts reported so far. This work not only provides a strategy to controllably fabricate specific defects in CS-SACs but also deepens the fundamental understanding on how pentagon defects regulate the electron structure and catalytic performance of metal-N 4 sites.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Zhitong Zhou,Weixiang Guan,Xiaoli Pan,Shengxin Zhang,Yang Su,Aiqin Wang,Tao Zhang
Synthesis of primary amines from alcohols is an economical and green route to access high-value N-compounds. However, challenges remain to develop both cost-effective and efficient catalysts. In this study, we developed a Ru-Co/ZrO 2 single-atom alloy catalyst which afforded diverse primary amines from alcohols in the presence of ammonia and hydrogen with exceptional conversion (up to 90%) and selectivity (80%) under mild conditions (0.7 MPa NH 3 , 0.3 MPa H 2 , 160 °C) and exhibited satisfactory stability upon regeneration. The turnover rate was approximately 8.4 times higher than that observed over the Co/ZrO 2 catalyst. Characterizations indicated that the alloyed Ru facilitated the reduction of Co, strengthened the interaction with H 2 and mitigated the over-strong adsorption of aldehyde intermediates. These combined effects contributed significantly to the enhanced catalytic performances. This work presents a promising strategy for the development of advanced catalysts in the amination of alcohols.
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Advanced Science
·
2022
·Vol. 9
·期 17
·2200518
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IF 17.521
Juan Meng,Zhihan Tong,Haixin Sun,Yongzhuang Liu,Suqing Zeng,Jianing Xu,Qinqin Xia,Qingjiang Pan,Shuo Dou,Haipeng Yu
An in-depth understanding of the electronic structures of catalytically active centers and their surrounding vicinity is key to clarifying the structure–activity relationship, and thus enabling the design and development of novel metal-free carbon-based materials with desired catalytic performance. In this study, boron atoms are introduced into phosphorus-doped nanoporous carbon via an efficient strategy, so that the resulting material delivers better catalytic performance. The doped B atoms alter the electronic structures of active sites and cause the adjacent C atoms to act as additional active sites that catalyze the reaction. The B/P co-doped nanoporous carbon shows remarkable catalytic performance for benzyl alcohol oxidation, achieving high yield (over 91% within 2 h) and selectivity (95%), as well as low activation energy (32.2 kJ mol −1 ). Moreover, both the conversion and selectivity remain above 90% after five reaction cycles. Density functional theory calculations indicate that the introduction of B to P-doped nanoporous carbon significantly increases the electron density at the Fermi level and that the oxidation of benzyl alcohol occurs via a different reaction pathway with a very low energy barrier. These findings provide important insights into the relationship between catalytic performance and electronic structure for the design of dual-doped metal-free carbon catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Xiaoping Xie,Kexin Wang,Xiaoyan Shen,Xu li,Su Wang,Shun Yuan,Bowen Li,Zhiwei Wang
Microplastics (MPs) have attracted widespread attention because they can lead to combined toxicity by adsorbing heavy metals from the environment. Exposure to lead (Pb), a frequently adsorbed heavy metal by MPs, is common. In the current study, the coexistence of MPs and Pb was assessed in human samples. Then, mice were used as models to examine how co-exposure to MPs and Pb promotes aortic medial degeneration. The results showed that MPs and Pb co-exposure were detected in patients with aortic disease. In mice, MPs and Pb co-exposure promoted the damage of elastic fibers, loss of vascular smooth muscle cells (VSMCs), and release of inflammatory factors. In vitro cell models revealed that co-exposure to MPs and Pb induced excessive reactive oxygen species generation, impaired mitochondrial function, and triggered PANoptosome assembly in VSMCs. These events led to PANoptosis and inflammation through the cAMP/PKA-ROS signaling pathway. However, the use of the PKA activator 8-Br-cAMP or mitochondrial ROS scavenger Mito-TEMPO improved, mitochondrial function in VSMCs, reduced cell death, and inhibited inflammatory factor release. Taken together, the present study provided novel insights into the combined toxicity of MPs and Pb co-exposure on the aorta. Environmental Implication Microplastics (MPs) and Lead (Pb) are pervasive in the environment, yet studies on the cardiovascular toxicity of MPs and Pb co-exposure remain scarce. This research investigates the effects of MPs and Pb co-exposure on aortic medial degeneration (AMD). The findings reveal the presence of MPs and Pb exposure in patients. Co-exposure to MPs and Pb accelerates AMD in the mice. Further experiments confirm that co-exposure to MPs and Pb affects vascular smooth muscle cell activity and inflammation by regulating the cAMP/PKA pathway and mitochondrial function. Our study offers new insights into the synergistic toxic mechanisms of MPs and Pb.
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PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Yang Haozhou,Guo Na,Xi Shibo,Wu Yao,Yao Bingqing,He Qian,Zhang Chun,Wang Lei
Cobalt phthalocyanine immobilized on carbon nanotube has demonstrated appreciable selectivity and activity for methanol synthesis in electrocatalytic CO 2 /CO reduction. However, discrepancies in methanol production selectivity and activity between CO 2 and CO reduction have been observed, leading to inconclusive mechanisms for methanol production in this system. Here, we discover that the interaction between cobalt phthalocyanine molecules and defects on carbon nanotube substrate plays a key role in methanol production during CO 2 /CO electroreduction. Through detailed operando X-ray absorption and infrared spectroscopies, we find that upon application of cathodic potential, this interaction induces the transformation of the planar CoN 4 center in cobalt phthalocyanine to an out-of-plane distorted configuration. Consequently, this potential induced structural change promotes the transformation of linearly bonded *CO at the CoN 4 center to bridge *CO, thereby facilitating methanol production. Overall, these comprehensive mechanistic investigations and the outstanding performance (methanol partial current density over 150 mA cm −2 ) provide valuable insights in guiding the activity and selectivity of immobilized cobalt phthalocyanine for methanol production in CO 2 /CO reduction.
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PubMed
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JOURNAL OF SOLID STATE CHEMISTRY
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2024
·
IF 3.2
Xiu-Zhen Yang,Tian-Qi Zhao,Renagul Abdurahman,Shi-Ji Liu,Yao-Xing Han,Yue Zhang,Xue-Bo Yin,Jie Gao
Fluorescence intensity ratio (FIR) technique demonstrates significant potential for non-contact temperature sensing with rapid response time, while the design of FIR probes is particularly intriguing. Herein, we report Pr–Al co-doped MgGa 2 O 4 persistent luminescence nanoparticles (PLNPs), as MgAl 0.04 Ga 1.96 O 4 : 0.1 % Pr 3+ (MAGP), for ratiometric temperature sensing application. Pr 3+ ions function as the emission centers for dual-emission at 612 and 494 nm, while Al 3+ ions adjust the lattice environment around Pr 3+ ions to enhance the luminescence. Consequently, 274 nm excitation induces the emissions at 494 and 612 nm, as the transitions of Pr 3+ for 3 P 0 → 3 H 4 and 1 D 2 → 3 H 4 , respectively. The emission mechanism is substantiated by density functional theory calculations, regarding the electronic transitions of Pr 3+ . Ratiometric temperature sensing is achieved over the temperature range of 303–573 K with the thermally non-coupled mechanism of the 3 P 0 / 1 D 2 energy levels by FIR at 612 and 494 nm, respectively. The maximum relative sensitivity was 0.91 %. The mechanism is corroborated as the non-thermally coupled energy levels through intervalence charge transfer. Thus, the reversible and sensitive response was illustrated for temperature measurement and the non-thermally coupled mechanism is efficient for the design of ratiometric temperature sensors.
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