ACS Catalysis
·
2026
·Vol. 16
·期 20
·20616-20627
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IF 13.6
Yuan Jingkang,Zhao Chao,Jin Yu,Hou Qilin,Cui Zhi,Tan Daolin,Ou Honghui,Yan Xiaoqing,Yang Guidong
The electrocatalytic co-reduction of nitrate (NO 3 − ) and carbon dioxide (CO 2 ) into urea represents a potential avenue for achieving efficient urea production. However, this process involves intricate C–N coupling reactions and faces a severe kinetic mismatch between the reduction pathways. This disparity typically leads to a disproportionate coverage of key C- and N-containing intermediates on the catalyst surface, resulting in dominant competitive side reactions. Herein, we report the design of a heterogeneous FeNi@AC catalyst that integrates isolated Fe single atoms and Fe–Ni dual-atom sites at the atomic scale, enabling the efficient conversion of NO 3 − and CO 2 into urea. Combined experimental and theoretical investigations reveal that the isolated Fe single-atom sites retain high nitrate reduction capability. Crucially, the introduction of Ni induces an electronic reconfiguration of the Fe center, which significantly lowers the energy barrier for CO 2 activation (from 0.7 eV to 0.1 eV). This activation effectively bridges the kinetic gap between C- and N-species. Consequently, the FeNi@AC catalyst achieves a urea yield rate of 13.6 mmol g –1 h –1 and a Faradaic efficiency of 51.7% at –0.8 V (vs RHE). This work not only presents an active catalyst for urea synthesis but also provides a site-specific regulation strategy for designing multifunctional atomic-site catalysts tailored for complex tandem reactions.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Lingchao Wang,Yun Guo,Xiaofan Li,Hui Guo,Yinzhong Liu,Xiaotao Zhu,Yiyu Qiao,Xuechun Yang
Developed a unique Gd-doped Tourmaline@MOF-ZnO nanostructure that integrates a polarized core with a highly porous shell. • Achieved a massive response (890.31 to 100 ppm), fast kinetics (34 s/18 s), and a ppb-level detection limit (56.63 ppb) for n-butanol at 240 °C under UV activation. • The gas-sensing performance is significantly boosted through the synergistic combination of the MOF-derived porous architecture, Tourmaline polarization, Gd-induced oxygen vacancies, and UV activation. Reliable monitoring of volatile organic compounds (VOCs) demands gas sensors with fast response, high sensitivity, and excellent selectivity. To this end, we designed a novel gas-sensing material based on a Gd-doped Tourmaline@MOF-ZnO core–shell nanostructure. This structure integrates a Tourmaline core with a porous MOF-derived ZnO shell, further enhanced via Gd doping. The gas sensing properties were evaluated under both dark condition and UV activation. At the operating temperature of 240 °C with UV activation, the optimized sensor with 0.08 wt% Gd and 5 wt% Tourmaline (denoted as 0.08 wt% Gd-5 wt% TML@ZnO) exhibited a remarkable response of 890.31 to 100 ppm n-butanol. This value is 9.96 times higher than that of the pristine MOF-derived ZnO (89.43). Moreover, the sensor demonstrated fast response/recovery times (34 s/18 s), high selectivity, excellent long-term stability, and a low detection limit of 56.63 ppb. The outstanding performance underscores the considerable promise of the optimized Gd-doped Tourmaline@MOF-ZnO core–shell composite for practical ppb-level VOCs monitoring. This work provides an effective strategy for designing high-performance gas sensors through the synergistic integration of rare-earth doping and core–shell structural design. Download: Download high-res image (214KB) Download: Download full-size image
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CHEMISTRY-A EUROPEAN JOURNAL
·
2026
·
IF 3.6
Meiqi He,Wei Zhang,Chengxin Zhu,Ying Liang,Wenjin Guo,Rong Chen
Electrochemical conversion of CO 2 and nitrate into urea offers a sustainable route for nitrogen fixation, yet the reliability of catalytic performance evaluation is frequently compromised by inaccurate product quantification. Current detection methodologies are susceptible to severe interferences from electrolyte pH fluctuations, byproduct accumulation (e.g., NO 2 − , NH 3 ), and complex electrolyte factors. In this study, we systematically decouple the interference mechanisms affecting these mainstream detection methods, revealing that extreme pH conditions lead to significant quantitative deviations in urease-based assays due to enzymatic denaturation. To overcome these limitations, we establish a comprehensive calibration strategy and a multi-method synergistic detection protocol. This approach integrates targeted pH optimization with a logic-guided selection of analytical techniques based on specific concentration ranges and impurity profiles. Validated using a BiOCl-catalyzed urea synthesis system, this integrated protocol demonstrates exceptional accuracy, stability, and cross-method consistency. By offering a standardized, high-throughput-compatible workflow for eliminating false positives and measurement errors, this work provides critical methodological support for the objective assessment of electrocatalytic urea synthesis. Graphical This study systematically evaluates matrix interferences in electrochemical C─N coupling for urea quantification. We define specific boundaries where ammonia and nitrite byproducts cause measurement deviations and elucidate the impacts of pH on detection methods. An integrated multi-method protocol is established and validated using a BiOCl catalyst, delivering a standardized workflow for the objective assessment of performance.
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ENERGY & FUELS
·
2025
·
IF 5.3
Hui Yang,Libo Han,Haiquan Su,Lili Wan,Yue Su
Dry reforming of methane (DRM) reaction has attracted much attention due to its important implications for the environment and energy. The nonprecious metallic nickel is a promising active metal in DRM catalysts because of its low price and high activity. However, nickel-based catalysts are prone to deactivation due to sintering and carbon deposition, which is the main factor limiting the industrial application of the DRM reaction. Herein, a highly stable DRM catalyst has been developed, which was a highly dispersed nickel-based catalyst Ni/N-C-DS (Ni supported on N–C support prepared by the double-solvent (DS) method), prepared by impregnating Ni2+ into the cavities of ZIF-8 using the double-solvent method (DS), followed by a one-step carbonization process. The results showed that the Ni/N-C-DS catalyst exhibited smaller metallic Ni nanoparticles, more dispersed Ni species, and richer pore structures. At a reaction temperature of 800 °C, the Ni/N-C-DS catalyst exhibited satisfactory DRM catalytic activity and stability, with CH4 and CO2 conversion rates reaching 82 and 85%, respectively. The H2/CO ratio approached 1, and no deactivation was observed during 300 h of continuous operation. A thorough study of the catalyst’s structure–activity relationship revealed that the high dispersion of Ni0 in the Ni/N-C-DS catalyst was the main source of high activity for the DRM reaction, while the high stability in the later stage (80–300 h) of the DRM reaction was mainly attributed to the synergistic effect between the in situ reduced Ni0 and the initially highly dispersed Ni0.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2025
·
IF 7.8
Mengcan Ju,Lili Yan,Zhiwen Cheng,Tiantian Li,Guanghui Li,Pinhua Rao,Qincheng Chen,Benjiao Huo
Persulfate-based advanced oxidation processes catalyzed by heterogeneous Fe-carbon composites represent a promising and competitive technology for the degradation of antibiotics. Herein, an environmentally friendly carbon material derived from tobacco stalk biomass was developed using potassium ferrate as both activator and Fe source, with urea serving as the N precursor. Magnetic N-doped biochar (H-Fe-N@BC) with abundant microporous-mesoporous structures and a high graphitization degree was obtained, and loaded Fe 3 N made the biochar with magnetism and simultaneously improved the ability of potassium persulfate (PS) activation in antibiotic-sulfamethazine (SMT) degradation. SMT (the initial pH≈7) could be degraded to 90.8 % within 15 min in the H-Fe-N@BC/PS system. In addition, H-Fe-N@BC maintained excellent catalytic activation performance under acidic and weakly basic conditions, and Cl - promoted the SMT degradation, while CO 3 2- and HPO 4 2- exerted inhibitory effects. The degradation mechanism by H-Fe-N@BC mainly consists of O 2 · − -dominated radical pathway as well as 1 O 2 and electron transfer-dominated non-radical pathway. Variation in composition of biochar and density functional theory calculation revealed that C O, graphite N, and Fe 3 N sites were crucial for activating PS to degrade SMT. These findings are of great significance by converting tobacco straw waste into high value-added biochar products with multiple active sites and applying them in the remediation of antibiotic-contaminated environment.
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Catalysis Science & Technology
·
2025
·
IF 4.2
Canyang Zhang,Yin Liang,Chao Chen,Wei Zhao,Bolong Li,Jianghao Wang,Zhenyu Zhang,Huiping Ji,Feng Zhou,Kaige Wang,Reinout Meijboom,Jie Fu
The decarbonylation of biomass-derived fatty acids (CnH2n+1COOH) presents a sustainable method for producing high-value alkenes (CnH2n). However, the development of efficient and highly selective catalysts for fatty acid decarbonylation remains challenging. In this work, we prepared a series of CoPhPhen/MWCNT-X catalysts by pyrolyzing a 4,7-diphenyl-1,10-phenanthroline (PhPhen) Co complex immobilized on multi-walled carbon nanotubes. In the model decarbonylation reaction of stearic acid, the optimized CoPhPhen/MWCNT-900 catalyst demonstrated remarkable catalytic efficacy, with 81.6% conversion of stearic acid and 58.3% yield of heptadecene. Characterization and comparative experiments demonstrated that the substantial phenyl groups in the PhPhen ligand engage in strong π-π interactions with the MWCNT, effectively inhibiting the migration and aggregation of cobalt single atoms during pyrolysis and thus maintaining a high density of active Co single-atom sites. Further electronic structure investigation revealed that the local electron density around the cobalt species markedly rises with higher pyrolysis temperatures, and this electronic impact exhibits a distinct positive association with the decarbonylation performance of catalysts. In situ DRIFTS was employed to reveal the adsorption and reaction process of fatty acids on the Co single-atom active sites: The fatty acid molecule first coordinates to the cobalt center via the carbonyl oxygen, followed by successive dehydration and decarbonylation processes, finally yielding H2O, CO, and olefins.
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ACS Omega
·
2025
·
IF 4.3
Songya Cui,Jiashuo Wang,Chengxiang Tian,Xiaoyu Xu,Dongxue Han,Guang Chen,Yufeng Yu,Liang Peng
Sodium-ion batteries (SIBs) are restricted in their energy storage capacity primarily because the considerable size of Na+ and inherently slow redox processes limit efficient charge transfer. Transition metal chalcogenides with layered structures have considerable promise as advanced materials of SIBs. Herein, the Ni-doped hollow MoS2/NC spheres with nitrogen-doped carbon are fabricated by a simple water/ethanol system combined with thermal annealing. Nickel doping effectively modifies the electronic properties of MoS2, leading to a substantial improvement in electrical conductivity and an increase in the density of electrochemically active sites. The addition of nitrogen-doped carbon within the composite helps to improve redox kinetics, ensuring improved structural integrity. Consequently, the Ni-MoS2/NC anode demonstrates excellent cycling stability, delivering a capacity of 176 mAh g–1 at 5.0 A g–1 for 10,000 cycles. Moreover, a full battery paired with a Na3V2(PO4)3/C cathode exhibits impressive rate performance, when the current is restored to 0.1 A g–1, and it showed a high specific capacity of 326 mAh g–1, which indicates that the Ni-MoS2/NC||Na3V2(PO4)3/C full battery exhibits robust performance across varying current densities, maintaining high electrochemical reversibility. This effective approach ensures improved electrochemical performance, prolonged cycling life, and higher efficiency, making hollow nanostructures a promising design for next-generation energy storage systems.
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PubMed
高影响因子
Journal of Hazardous Materials Advances
·
2025
·
IF 7.7
Shiyu Cao,Furong Guo,Meiqi Li,Xin Zhang,Yifu Xu,Jiangshan Li
Roxarsone (ROX), a widely used organic arsenic feed additive, enters paddy soils through animal manure fertilizer, posing serious risks to environmental and human health. However, the underlying mechanisms of ROX stabilization, particularly the role of soil cultivation duration, remain poorly understood. Here, we compared ROX stabilization in new paddy soil (NPS, 10-year cultivation) and old paddy soil (OPS, 100-year cultivation). NPS exhibited higher ROX stabilization ability than OPS, as evidenced by a 1.5-fold higher adsorption rate constant, a 28-fold higher organic carbon-normalized partition coefficient (K oc ) and retention of 13-fold more arsenic in the residual fraction (non-extractable arsenic). The improved adsorption and stability in NPS were mainly due to complex formation between nitrogen-rich organic matter and Fe(II). In-situ spectroscopic and electrochemical analyses revealed that the complex promote ROX fixation by forming a Fe(II)-ROX-N ternary configuration. This structure was derived from the bidentate binuclear binding of As(V) with iron sites and deprotonated N-containing functional groups. These findings provided mechanistic insights into organic arsenic adsorption in soils and offered theoretical guidance for optimizing soil composition management strategies.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Feihong Zeng,Fangyuan Zhao,Xinyu Su,Qiang Wang,Zhibo Liu,Chao Zhen,Yong Liu,Gang Liu,Wencai Ren,Gaorong Han,Zongping Chen
Constructing p-n homojunctions while confining them on the surface of two-dimensional (2D) photocatalyst is a highly promising way to promote charge separation and thus improve the photocatalytic performance, yet they have rarely been achieved thus far. Here, we prepare 2D titanium oxide nanosheets enriched with both n-type oxygen vacancies and p-type titanium vacancies that form surface localized p-n homojunctions. The built-in electric field of the homojunctions promotes the unidirectional movement and separation of photogenerated carriers. Moreover, the p-n homojunctions confined to the surface of the ultrathin nanosheet can interact directly with the reactants, which reduces the recombination probability of electron-hole pairs. As a result, these p-n homojunctions enable an outstanding photocatalytic activity for water decontamination which is 30 times higher than that of benchmark titanium oxide. These results provide new opportunities for design and engineering of defects of 2D photocatalysts, potentially driving technological breakthroughs for energy conversion and environmental remediation.
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DYES AND PIGMENTS
·
2025
·
IF 4.2
Tingye Gu,Qing Guo,Dongming Qi,Pu Gao,Weiguo Chen,Zhihua Cui,Sateesh Bandaru
N -hydroxysuccinimide esters (NHS esters) are widely recognized as amine-reactive compounds due to their mild reaction conditions and high efficiency. In this study, NHS ester group was introduced into the dye chromophores to design and synthesize carboxylic acid succinimidyl ester dyes ( CSED s) in red, yellow and blue colors. The CSED s were characterized using high-resolution mass spectrometry, proton nuclear magnetic resonance, and infrared spectroscopy. When the NHS ester group was introduced, UV–vis absorption spectroscopy only slightly affected the molar extinction coefficient and maximal absorption wavelength. Hydrolysis studies demonstrated that CSED s hydrolyzed slowly in acidic environments but quickly in weakly alkaline ones, with near-complete hydrolysis taking place at pH 8.5 after half an hour. It was discovered that CSED s could successfully dye silk fibroin at room temperature in weakly alkaline conditions, producing a high color depth and more than 95 % color fixing. The binding of CSED s to silk fibroin was confirmed through covalent bonds using DMF stripping method and dialysis method. Furthermore, the color fastness of dyed silk fibroin to washing and rubbing was rated above grade 4–5. Compared to commercial dyes, the milder dyeing conditions of CSED s can save energy and did not require a significant amount of salt to promote the dyeing process.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Zhikuan Liu,Quan Diao,Ziyang Zheng,Heng Liu,Muen Yang,Genxing Zhu,Xueling Wu,Yuanyuan Li,Xiumei Xu,Quan Huang,Mingli Jiao
Lanthanum (La) was incorporated into modify α-Fe 2 O 3 porous nanosheets via the smoldering solvothermal combustion method, and applied to establishing a gas sensor with high responsivity and rapid recovery. Material characterization revealed successful synthesis of the α-Fe 2 O 3 porous nanosheets with uniform incorporation of La. The introduction of La modulated both the morphology and pore size of the α-Fe 2 O 3 nanosheets, while also enhancing the oxygen vacancy content and specific surface area. Gas sensitivity testing demonstrated that the modified α-Fe 2 O 3 porous nanosheets exhibited superior gas-sensitized properties. Specifically, the Fe 2 O 3 /La-5 % exhibited a response of 81.55–100 ppm n-butanol at 275 °C, which was 8.43 times higher than that of pure α-Fe 2 O 3 (response value of 9.67), as well as excellent selectivity, fast response and recovery. Further analysis using UV-Vis spectrophotometry and electrochemical testing elucidated the mechanism underlying the enhanced gas-sensing performance, indicating that La doping influenced the microstructure and oxygen vacancy concentration of Fe 2 O 3 . The green, straightforward, and cost-effective synthesis method, coupled with the excellent gas-sensing performance, provides a theoretical basis for the advancement of high-performance n-butanol sensors.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Jihui Yao,Lijuan Su,Lipeng Guo,Xing Wu,Haibo Zhu
N -ethylcarbazole, as a liquid organic hydrogen carrier, has shown great promise in the field of hydrogen storage technology. The development of efficient and stable catalyst for producing H 2 through N -ethylcarbazole dehydrogenation is crucial for its practical application. In this study, a series of mesoporous Al 2 O 3 -supported Pt catalysts with K modification were developed for N -ethylcarbazole dehydrogenation. These catalysts were characterization using various techniques including XRD, N 2 adsorption–desorption, TEM, 27 Al MAS NMR, XPS, NH 3 -TPD, H 2 -TPR, CO-FTIR, and Py-IR, providing detailed structural information to elucidate the structure–activity relationship. Mesoporous Al 2 O 3 was found to possess significant amounts of coordinatively unsaturated pentacoordinate Al 3+ , which greatly promotes the dispersion of Pt species for the formation of small Pt particles. The addition of K was observed to modulate the electronic structure of Pt, reduce the acidity of the catalysts, and inhibit the sintering of Pt. These synergetic effects led to Pt 3.0 /K 3.0 -Al 2 O 3 -m achieving remarkable performance in dodecahydro- N -ethylcarbazole dehydrogenation at 180 °C and 101 kPa, delivering a dodecahydro- N -ethylcarbazole conversion of 100 %, H 2 release amount of 5.63 wt% and dehydrogenation efficiency of 97.10 %. Additionally, this catalyst demonstrated high efficiency in the dehydrogenation of dodecahydro- N -propylcarbazole, octahydro-2-methylindole, and octahydro-1,2-dimethylindole, achieving dehydrogenation efficiencies of 99.60 %, 100 % and 100 %, respectively. These findings provide valuable knowledge for the rational design of efficient metal-based catalysts for liquid organic hydrogen carriers in hydrogen storage systems.
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