AICHE JOURNAL
·
2025
·
IF 4
Bo Wang,Shuangjiang Li,Xiandong Hao,Wenbo Zhao,Zhiyong Xu,Yongming Luo
Traditional amine scrubbing for SO 2 capture typically dilutes alcohol amines with water to improve mass transfer, resulting in high volatility and desorption energy consumption. Inspired by the exceptional properties of ionic liquid (IL) 1-ethyl-3-methylimidazolium thiocyanate ([EMIM][SCN]), we herein propose substituting water with [EMIM][SCN] in a novel SO 2 absorbent system based on N -methyl ethanolamine (MDEA). MDEA acts as the primary SO 2 absorbent, while [EMIM][SCN] serves as an auxiliary absorption component and physical properties regulator. Performance evaluations reveal that MDEA-[EMIM][SCN] achieves high thermal stability (~483.15 K), low viscosity (~26 mPa s), excellent absorption capacity (~1.64 mol/kg at 298.15 K and 2000 ppm SO 2 ), high SO 2 /CO 2 selectivity (~101), and low desorption energy (approximately −95.6 kJ/mol). Thermodynamic modeling illustrates MDEA and [EMIM][SCN] contribute independently to absorption. Optimal energy consumption was determined by the proposed objective function. This work exemplifies the non-aqueous alkanolamine/IL system for SO 2 capture, offering a promising approach for developing efficient, low-energy SO 2 absorbents.
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JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Zhigang Yi,Xiangnan Chen,Zhenhua Dong,Ruohao Li,Qiong Tang,Xin Tian
The low efficiency and insufficient long-term cycling stability under high current density remains one of the bottleneck issues restricting the development of vanadium flow batteries. Based on the integrated ‘rigid-flexible’ characteristics, carbonized polypyrrole/polyvinylpyrrolidone interlaced architectures are constructed on the carbon felts to synergistically enhance the electrochemical activity and long-term cycling stability. The modified electrode (N-NCF) achieves a specific surface area of 11.98 m 2 /g, which is 6.34 times that of the pristine carbon felt (PCF). Under 280 mA cm −2 , N-NCF maintains an energy efficiency of 73.1 %, representing a 5 % improvement over PCF. Furthermore, the nanofiber-interlaced architectures enable N-NCF to exhibit exceptional long-term cycling stability. After over 10,000 cycles under 280 mA cm −2 , the energy efficiency remains 66.4 %, with an extremely low decay rate of 0.000899 %. The optimized N-doping and nanofiber-interlaced architectures synergistically enhance the electrochemical activity and stability of the carbon felts, thereby establishing a long-term stable electrochemical catalytic network. This work provides referencing strategies for the stable electrodes of vanadium flow batteries.
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Catalysis Science & Technology
·
2025
·
IF 4.2
Fuwei Gan,Wen Liu,Xinbao Zhang,Maochen Qian,Shaoguo Li,Yuzhong Wang,Junjie Li,Xiangxue Zhu,Xiujie Li
Primary amines, exemplified by n-butylamine, serve as critical intermediates in the synthesis of pharmaceuticals and agrochemicals. Amination of n-butanol with ammonia over supported cobalt catalysts represents a promising synthetic route. To enhance the catalytic performance of Co-based amination catalysts, we reported an acid-treated strategy that allows for precise regulation of cobalt speciation. Among the evaluated supports, silicalite-1 demonstrated superior amination performance, attributed to its unique ability to enhance cobalt dispersion and suppress acid-induced side reactions. Through acid treatment, oversized Co3O4 nanoparticles are selectively removed, thereby preserving highly dispersed cobalt species. Under rigorous reaction conditions (WHSV = 2.5 h-1), the acid-treated catalyst achieved 90% selectivity toward n-butylamine, accompanied by improved stability compared to untreated counterparts. Mechanistic investigations revealed that well-dispersed metallic Co0 nanoparticles promoted selective C-N bond formation via efficient coupling, whereas larger cobalt domains facilitated dehydrogenation-driven carbon deposition pathways. This work establishes a clear structure-performance relationship for cobalt-based amination catalysts, offering a blueprint for sustainable amine production.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2025
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IF 5
Nusrullah Mehtab,Lu Bin,Miao Guilan,Bibi Amna,Wang Yanmei
Acrylamide-based non-ionic polymers have gained significant attention for wastewater treatment due to their high flocculation efficiency. However, optimizing the polymer dosage and knowing the role of hydrogen bonding in flocculation remain challenging. In this study, acrylamide/(N-hydroxyethyl)acrylamide (AM/HEA) copolymers at different molar ratios were synthesized via solution polymerization. The polymers were characterized using FTIR, 1 H NMR, DSC, and TGA. The kaolin suspension was employed to evaluate the flocculation performance of copolymers by the jar test method. The AM/HEA copolymers showed superior flocculation efficiency, achieving 98% turbidity removal at an optimal polymer flocculant dose of 0.2 mg/L, with a stirring speed of 400 rpm and a stirring time of 180 s. Zeta potential and TEM imaging results showed that flocculation primarily occurred through polymer adsorption on the kaolin surface, with its coiled conformation may enhance particle bridging. These results emphasize the critical role of polymer molecular structure in optimizing flocculation performance and suggest AM/HEA copolymers as efficient flocculants for water treatment exercises.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Huaqi Zhang,Siyi Chen,Zhenhao Wang,Chaoran Fan,Tianming Li,Na Yan,Yian Zheng
Semi-coke (SC), a solid waste generated from the dry distillation of oil shale, is rich in organic matter, classifying it as a functional carbon-based material. Combining the progressive advantages of functionalized carbon-based materials in advanced oxidation technology, this study prepared Fe-N co-doped semi-coke (Fe-N-SC) through a facile one-step pyrolysis of SC pre-impregnated with potassium ferricyanide. Under visible light (VIS) irradiation, Fe-N-SC was able to activate periodate (PI) to establish an Fe-N-SC/PI/VIS system for degrading norfloxacin (NOR). The results showed that this system achieved 99.5%-NOR removal, with a mineralization degree of up to 68.6%- within 30 min. Furthermore, Fe-N-SC exhibited stable performance over a wide pH range (3−9) and maintained high NOR removal efficiency in real water matrices, indicating its robustness and practical applicability. Electron paramagnetic resonance and free radical quenching experiments revealed that h + and ·OH were the primary species responsible for NOR degradation in Fe-N-SC/PI/VIS system. The proposed mechanism involved reactive oxygen species-driven oxidative cleavage of piperazine ring in NOR, leading to its stepwise breakdown and mineralization into harmless end-products. During the degradation process, no toxic intermediates were detected, highlighting the environmental safety of Fe-N-SC/PI/VIS system for sustainable and highly effective removal of antibiotics from aquatic environment.
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Molecular Catalysis
·
2024
·
IF 3.9
Pengcheng Wang,Qingqing Jiang,XingYu Li,Xuedong Wang,Juncheng Hu
Generally, researchers focus on the regulation of metal sites rather than surrounding nonmetals in photothermal CO 2 hydrogenation reaction. Herein, concerning the role of non-metallic N species, a series of Co/NC-T catalysts have been fabricated via high-temperature pyrolysis of Zeolitic Imidazolate Frameworks-67. The CO 2 conversion rate shows a consistent tendency with the ratio of graphitized-N species while the product selectivity is closely related to the coordination state of Co-N x species. Co/NC-800 catalyst achieves high CO 2 conversion rate of 758 mmol g cat -1 h -1 with CH 4 selectivity of 99.6 %. After adding extra graphitized-N species, the CO 2 conversion rate could further enhance to 80.2 % for N-Co/NC-2. The role of N species in photothermal CO 2 hydrogenation reaction has been investigated in details, providing new insights for the design of metal organic frameworks derived metal/N-doped carbon catalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Xiang Li,Danwen Guo,Shanying He,Jiahao Kang,Yijuan Zhao,Shaohua Wu,Chunping Yang
Peroxymonosulfate-based advanced oxidation processes (PMS-based AOPs) via nonradical pathways have attracted close attention due to their excellent anti-interference properties and high selectivity in degrading organic pollutants from wastewater. However, the highly efficient production of nonradicals for PMS activation remains challenging, especially for recalcitrant organic pollutants such as tetracycline (TC) in complex aqueous matrices. Here, MnO and nitrogen-doped carbon catalysts were synthesized using NH 4 Cl modified strategy. The performances and mechanisms of TC degradation were evaluated, and toxicity of the system was also assessed. Results showed that the system achieved 86.7 % removal of TC within 30 min with a rate constant of 0.1713 min −1 . This system demonstrated effective TC degradation across a broad pH range (3.0–10.5) while exhibiting resistance to diverse anionic interferences in aqueous matrices. Characterization data showed that NH 4 Cl calcination led to a hierarchical porous structure with optimized MnO dispersion and nitrogen functionality in the carbon support, further significantly enhancing nonradicals generation through PMS activation. The key active sites were identified as Mn-N X sites, graphitic nitrogen, and C-O/C-N groups. Quenching experiments and ESR tests indicated that electron transfer and Mn(V) played the major role in TC degradation, followed by singlet oxygen ( 1 O 2 ). Based on LC-MS analysis of intermediates, three primary TC degradation pathways were identified: hydroxylation-driven ring-opening, oxidative demethylation/deamination, and oxidative ketonization. Toxicity assessment via the Toxicity Estimation Software Tool confirmed a significant reduction in ecotoxicity throughout these pathways. These data could be referred for the optimization of PMS-based AOPs in wastewater treatment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
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IF 21.1
Yuhou Pei,Di Li,Yufeng Pei,Zongmiao Li,Yuting Liu,Xiang Ling,Yingying Lu,Bing Zhang
Urea synthesis by co-electroreduction of CO 2 and nitrate provides a promising strategy for sustainable fertilizer production. Despite advances in catalyst exploration, it is of significance to figure out the microenvironment on the electrode interface toward the kinetically matched C-N coupling. Here, we fabricated a hydrophobic triple-phase catalytic interface through a simply blending of commercial CuZn alloy and polytetrafluoroethylene (PTFE) particles for proof of concept. Incorporating PTFE boosted the Faradaic efficiency of urea from 8 % to 49 % and tripled the urea production rate. Kinetics and in-situ spectra studies reveal that hydrophobicity slows the proton/electron transfer during nitrate reduction, accelerates CO₂ diffusion at the triple-phase interface, and preserves high-valent asymmetric adsorption sites. This synergy extends the lifetime and surface coverage of critical C-/N-intermediates, and thus kinetically-matched asymmetric C-N coupling.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 24
·2313719
·
IF 18.5
Yingchao Wei,Zheng Ma,Wang Li,Chengjun Li,Boyu Yang,Chengwei Sun,Shuangfu Gang,Wenguang Zhang,Hui Long,Xin Li,Qinghui Jiang,Dan Zhang,Yubo Luo,Junyou Yang
Exploring N-type High-entropy materials with both high thermoelectric and mechanical properties is highly desirable for all-high-entropy thermoelectric generators (TEGs) since the thermoelectric and mechanical properties of N-type one are largely behind its P-type counterparts. Herein, a new rock-salt structure N-type high entropy thermoelectric AgBiPbSe 2 S is introduced with a bandgap of ≈0.43 eV. The atomic radii difference of each component results in a large lattice distortion of 0.246, leading to a low thermal conductivity of 0.36 W m −1 K −1 at 823 K. The figure of merit ( ZT ) reaches 0.6 for AgBiPbSe 2 S at 823 K. Moreover, Ag 2 Se precipitates are included in AgBiPbSe 2 S to filter low energy carriers for high Seebeck coefficients and to scatter phonons with nanoscale wavelength for ultralow lattice thermal conductivities. Consequently, a peak ZT of ≈1.18 at 823 K and an average ZT of 0.60 at 400–823 K are obtained for Ag 1.02 BiPbSe 2 S. More importantly, high mechanical properties are also obtained in Ag 1.02 BiPbSe 2 S, of which the Vickers hardness and flexural strength are ≈209 Hv and 32 MPa, respectively, originating from the enhanced lattice friction by chemical short-range disorder (i.e., high entropy effect) and dispersion strengthening caused by Ag 2 Se nanoprecipitates.
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ACS Applied Nano Materials
·
2025
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IF 5.5
Mingming Du,Anxian Peng,Hongyue Liu,Huimei Chen,Qiyun Li,Zheng Fang,Ganning Zeng,Rongjun Yan
The well-designed internal electric field (IEF) with band bending effects will effectively accelerate the separation and transfer of photogenerated charges to foster a photocatalytic performance. Hence, in this work, the IEF-induced BiOCl/TiO2 p-n heterojunctions are prepared through the hydrothermal method for photocatalytic H2O2 production. The BiOCl/2TiO2 composite performed a superior H2O2 yield of 4.75 mM h–1, which is 4 times higher than that of pristine BiOCl. The p-n heterojunction mechanism was investigated via XPS and photoelectrochemical property tests, in which BiOCl/2TiO2 showed the highest photogenerated charge separation efficiency for boosting photocatalytic activity. This work provided an effective strategy for the design of p-n heterojunction photocatalysts to enhance photocatalytic performance.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Hanjun Zhang,Jing Chen,Yuxin Shi,Yaoyue Yang,Xiaole Jiang
Regulating the local microenvironment of metal centers represents an effective yet challenging approach to enhance the catalytic performance of atomically dispersed transition metal-nitrogen-carbon (M–N–C) catalysts towards the oxygen reduction reaction (ORR). Herein, atomically dispersed Cu–N–C catalysts featuring with adjustable carbon vacancies/defects concentrations (Cu–N–C V –X) are fabricated using a simple molten-salt-assisted pyrolysis strategy. The optimized catalyst (Cu–N–C V -1000) exhibits superior ORR catalytic performance with a half-wave potential ( E 1/2 ) of 0.89 V versus the reversible hydrogen electrode (RHE) and a turnover frequency ( TOF ) of 5.01 e site -1 s −1 at 0.85 V, surpassing Pt/C and most recently reported single-atom catalysts. Theoretical calculations confirm that defects adjacent to Cu–N 3 site downshift the d-band center of active sites, facilitating the desorption of *OH intermediate and thereby significantly enhancing the ORR kinetics. Consequently, the Cu–N–C V -1000-based zinc-air battery (ZAB) delivers a peak power density of 175.0 mW cm −2 along with a high discharge specific capacity of 819.4 mA g -1 Zn . This work confirms that the deliberate creation of suitable defects is an effective approach to optimize the intrinsic ORR activity of atomic M–N x sites, providing new insights into the rational design of high-performance catalysts for practical metal-air batteries.
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DIAMOND AND RELATED MATERIALS
·
2025
·
IF 5.1
Jinghui Xun,Zerui Chen,Aiyun Meng,Le Huang,Shuzhang Niu,Shaozhong Zeng,Xiao Yu,Weifeng Liu,Dongju Fu,Xuguang Liu
The scarcity and poor cycle stability of platinum, the key catalyst for the oxygen reduction reaction (ORR) in fuel cells and metal-air batteries, necessitate the development of alternative catalysts that are low-cost yet highly efficient. In this study, a novel catalyst was synthesized through chemical activation and nitrogen doping of distillers' grains, a biomass material that is rich in heteroatoms. Under alkaline conditions (0.1 M KOH), the ORR peak potential (0.833 V) of the resulting catalyst is comparable to that of commercial Pt/C (0.844 V), with a half-wave potential(E 1/2 ) of 0.802 V, achieving 97.3 % of the Pt/C performance. The onset potential (E onset ) of 0.93 V is also close to that of Pt/C (0.94 V). When the catalyst loading is increased to 0.75 mg/cm 2 , it exhibits a similar current density, E 1/2 of 0.81 V, and E onset of 0.98 V, even surpassing Pt/C. Stability tests using the i-t method show a current decay of 23.96 % after 12 h, outperforming the 79.71 % decay observed for Pt/C. Furthermore, the catalyst demonstrates superior methanol tolerance. In addition to providing a new way to utilize distillers' grains, the new catalyst achieves catalytic properties comparable to commercial Pt/C catalysts while controlling costs, and is expected to be a potential alternative to Pt/C catalysts for applications.
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