Molecular Catalysis
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2025
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IF 4.9
Binxin Lv,Jiayue Yu,Fengchen Zhou,Zizi Wang,Junjun Zhang,Yifan Zhang,Yang Wu,Yong Wang,Wen Luo
Urea electrosynthesis plays a vital role in the nitrogen cycle, promoting carbon neutrality while also being energy-efficient. However, the complexities involved in the simultaneous of carbon and nitrogen-containing species significantly hinder the selectivity and yield of urea. In this study, we report a CuZn bimetallic catalyst that is capable of converting CO 2 and NO 3 ⁻ into urea, with a maximum Faraday efficiency of 40% at -0.6 V vs. RHE, alongside an impressive urea yield rate of 304.8 mmol h ⁻¹ g cat ⁻¹ at -0.9 V vs. RHE, surpassing the performance of both monometallic Cu and Zn catalysts. In situ spectroscopic analysis demonstrates that the Cu sites within CuZn facilitates the adsorption and activation of CO 2 and NO 3 ⁻ , while Zn sites additionally facilitate CO 2 adsorption and reduces the adsorption strength of *CO and *NH 2 on the catalyst surface, collectively promoting the formation of *CONH 2 as a key intermediate in urea synthesis. This study highlights the unique role of zinc in urea synthesis, offers new insights into optimizing the performance of copper-zinc catalysts, and serves as a valuable reference for future research on the role of zinc in urea synthesis.
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ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Lanlan Yu,Jincheng Mu,Huiling Liu,Gang Liao,Boyi Li,Yufen Xia,Zhimin Wang,Jili Yuan,Jiachao Shen,Chengbin Liu
Electrocatalytic nitrate reduction into ammonia (NitRR) over Co-based catalysts is attractive but still constrained by the competition with H* coupling to produce H 2 . Additionally, the fundamental mechanism underlying the interfacial engineering associated with electronic state transformation for strengthening oriented NitRR remains elusive. Herein, a Co(OH) 2 /Bi 12 O 17 Br 2 heterostructure is fabricated using a one-step wet chemistry method, performing remarkable reactivity for NH 3 production own to the formation of electron-deficiency Co sites induced by Bi 12 O 17 Br 2 . Unexpectedly, the NitRR activity of Co(OH) 2 /Bi 12 O 17 Br 2 increases gradually in the initial stage and then keeps at a high level, which is uncovered as the reconstruction of Bi 12 O 17 Br 2 into Bi 0 . Theoretical calculations suggest that the in situ reconstruction guides the electron-deficiency of Co and the shift of d -band center of Co toward the Fermi level, thus promoting the adsorption and conversion of intermediates. The synergistic effect of the hydrolysis dissociation over Co(OH) 2 and the inhibition of H* coupling over Bi 0 contributes to high selectivity and activity for NitRR. The reconstructed catalyst shows a high ammonia yield rate of 7343.3 µg h −1 mg −1 at −0.6 V versus RHE and nearly 100% Faradaic efficiency at −0.4 V versus RHE. This study provides insight into the strengthening mechanism of Co-based catalysts for NitRR.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Shuangquan Zhao,Renxin Li,Jingquan Wang,Erdeng Du,Jinyan Yang,Hongguang Guo
Binding effects of dissolved organic matter (DOM) to antibiotics on redox processes have received much attention. However, most studies have focused on the role of humic acid (HA) in homogeneous systems, its binding interactions with antibiotics within carbon-based persulfate (PS) activation systems remain poorly understood. This study addresses this knowledge gap by investigating the impact of HA complexation on sulfonamide antibiotic degradation within a model CNT-CO 2 /PS non-radical system. The fluorescence quenching effect and ultraviolet visible spectral shifts of HA confirmed its binding effect with sulfonamide antibiotics. When the binding effect occurred, the degradation rate of the system for sulfamethoxazole increased by 21.5% compared with that of unbound, the degradation rate of sulfadiazine decreased by 15.9%, while sulfamerazine and sulfapyridine remained basically unchanged. Electrochemical impedance spectroscopy and Tafel analysis identified the CNT-CO 2 nano-interface as the primary site for electron transfer. Furthermore, cyclic voltammetry and linear sweep voltammetry revealed that the electron transfer intensity between the CNT-CO 2 /PS system and pollutants changed significantly when the binding effect occurred. By building a theoretical computational model of HA with sulfonamide antibiotics, the changes before and after binding was also examined. Consequently, the binding effect of HA affected the degradation rates primarily by modifying the direct electron transfer capacity between the CNT-CO 2 /PS system and sulfonamide antibiotics. This study elucidates a key mechanism, modulation of direct electron transfer by HA complexation, governing sulfonamide antibiotic fate in advanced carbon/persulfate oxidation processes.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Guan Sheng,Yudong Jiang,Zirong Yan,Jinshu Tian,Shaobo Tu
MXenes represent exceptionally promising electrocatalytic materials for ammonia synthesis, owing to their outstanding electrical conductivity, modifiable surface functional groups, exceptional hydrophilicity, high specific surface area, and electronegative surface characteristics. In this investigation, we systematically demonstrate that the persistent challenge of Cu and Co nanoparticle agglomeration can be effectively addressed through the in-situ growth of bimetallic CuCo nanoparticles on Ti 3 C 2 T x MXene nanosheets. This innovative approach significantly enlarges the electrochemically active surface area, maximizes the exposure of catalytically active sites, and optimizes mass transport properties, consequently leading to substantially enhanced electrocatalytic performance for ammonia synthesis. Among the series of Cu x Co y /MXene composites developed, the Cu 2 Co 1 /MXene hybrid catalyst demonstrates superior nitrate reduction reaction (NO 3 RR) activity, achieving remarkable performance metrics including: An exceptional ammonia yield rate of 2.73 mg cm −2 h −1 at an applied potential of −0.85 V versus RHE, a high Faradaic efficiency of 72.05 %, and outstanding selectivity reaching 90.6 %. These breakthrough results establish new benchmarks for MXene-based electrocatalysts in sustainable ammonia production.
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ANALYTICA CHIMICA ACTA
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2025
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IF 6
Ying Gao,Haiqin Li,Xiaochun Li
Background Urinary tract infection (UTI) is a significant global health issue. Urine bacterial culture is time-consuming, prone to misdiagnosis, and the existing sample pretreatment methods are cumbersome, relying on centralized laboratories and specialized equipment. Colorimetric sensing provides a faster alternative. However, its accuracy is often compromised by the variable color of the patient's urine samples. Therefore, it is clear that a rapid, simple, gentle, and environmentally friendly pretreatment method is needed that effectively eliminates color interference in colorimetric detection and is compatible with smartphones, enabling real-time, quantitative on-site monitoring of UTI. (90) Results In this study, we describe a unique smartphone-assisted diagnostic method for quantifying nitrite, leucocyte esterase (LE), and bacteria in urine samples. The method employs activated carbon composite hydrogel spheres for urine pretreatment, which effectively removes background color interference and improves sensor performance, and combined with a smartphone-based microplate analyzer independently developed by our group previously, allows for precise colorimetric examination. This will aid in the prompt detection and dynamic monitoring of urinary tract infections in clinical settings. Furthermore, the bacterial detection time was shortened to 2 h, enhancing the accuracy and timeliness of the diagnostic process. The detection limits of nitrite, LE, and E. coli were 0.0584 mg L-1, 0.0775 Leu μL-1, and 2.94 CFU mL-1, respectively, meeting clinical requirements. Validation of 147 clinical samples indicated high consistency with the Sysmex UC-3500 Automatic Urine Analyzer, demonstrating the sensor's durability and accuracy. (141) Significance Activated carbon hydrogel beads with high adsorption properties were used for the pretreatment of urine samples for the first time, effectively removing background color interference in colorimetric detection. Integration of a smartphone-based microplate analyzer with a hydrogel slow-release system enables quantitative detection of nitrite, LE, and bacteria. This strategy offers a portable, low-cost solution for home-based UTI monitoring, enabling more timely management and appropriate administration of therapy to improve patient outcomes. (71)
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