WASTE MANAGEMENT
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2024
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IF 7.1
Jing Gao,Wenchao Lu,Yujiang Li,Tao Wu
This article employs six organic acids to selectively dissolve Mo, Ni and V from spent catalysts, and the most effective acid is identified. Then, the effects of key leaching parameters, including acid concentration, temperature, and S/L ratio, on metal leaching are systematically explored to determine the leaching mechanism. The results demonstrate that the leaching ability of organic acids followed the order: oxalic acid > citric acid > tartaric acid > malonic acid > acetic acid > formic acid. The leaching process of metals was jointly influenced by acidolysis and complexolysis. Among them, more than 93.07 % of Mo, 86.64 % of V, and 74.21 % of Ni were selectively leached with oxalic acid at the optimum condition: S/l: 1/20, oxalic acid: 1.0 mol/L, temp: 60 °C. From the correlation coefficients, the resulting activation energies, and n values, it was demonstrated that Mo and V followed the Avrami dissolution reaction model, V leaching was controlled by the diffusion mode, and Mo leaching was controlled by a mixed mode of chemical reaction and diffusion. The dissolution behavior of both metals consistently adhered to the linear trend of the Avrami kinetic model under varying S/L ratios and oxalic acid concentrations.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Ruoyu Wei,Mansheng Liao,Lidan Sun,Qingfeng Zhang,Hong Zhang,Lei Zhang,Zhongxin Song
Developing highly efficient and low-cost bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in water splitting poses significant challenges. In this study, a novel bifunctional electrocatalyst, Irn-CoMoPOx, was achieved via incorporating low-loading Ir single atoms and clusters with the high-valence Mo6+ modified CoPOx nanosheets. The Irn-CoMoPOx catalyst demonstrates remarkable low overpotentials of 222 mV and 36 mV for the OER and HER, respectively, in delivering a current density of 10 mA cm–2. When employed as both the anode and cathode catalyst in overall water splitting, the Irn-CoMoPOx∥Irn-CoMoPOx configuration exhibits a superior cell voltage of 1.53 V, outperforming the benchmark Pt/C∥IrO2 electrolytic cell (1.60 V) for achieving the current density of 10 mA cm–2. Benefiting from the high-valence of Mo species, the metal–support interaction of Irn-CoMoPOx was greatly strengthened, resulting in an order of magnitude increase in the mass activity of Ir for the HER. The high valence of non-noble metals plays a crucial role in tuning the local electronic configurations and optimizing the adsorption energies of the intermediates, which synergistically improves the overall performance of Ir in water splitting. The study provides valuable insights for future research in the utilization of Ir-based bifunctional catalysts for overall water electrocatalysis applications.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Hengyuan Liu,Yingzhe Liu,Xuecheng Zeng,Xude Yu,Jianhong Xu
Electrocatalytic nitrogen reduction reaction (ENRR) is emerging as a promising routine for the sustainable production of ammonia. Hindered by the strong triple bond in N2 and unfavorable hydrogen evolution reaction, it is critical to develop efficient catalysts with excellent activity and selectivity. Herein, we propose a novel microfluidic platform that achieves the continuous synthesis and morphology regulation of a two-dimensional heterocatalyst FeMo/g-C3N4 through a precipitation process in a confined space. Owing to the rapid mixing and microfluidic manipulation, FeMo/g-C3N4 maintains an overwhelmingly favorable structure compared to the batch methods. Benefiting from the ultrasmall active sites (0.86 nm), homogeneous nanodot distribution, and abundant 2D surface, the promoted N2 chemisorption and competitive ENRR performance can be simultaneously ensured, as confirmed by the experimental studies. By varying the applied working potential, the optimal ammonia yield can be determined as 33.25 μg h–1 mgcat.–1 at −1.2 V. This work innovatively opens a pathway for morphological fine structural tuning of two-dimensional heterocatalysts, further promoting the ENRR field’s development.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yanxu Wang,Lijia Huang,Tian C. Zhang,Yan Wang,Shaojun Yuan
Ammonia gas (NH 3 ) is a notorious malodorous pollutant with detrimental effects on environment and human health. Removing NH 3 through photocatalytic oxidation remains a challenging task due to unclear reaction mechanisms. In this study, DFT simulation results revealed that C doped TiO 2 could extend the photo-response range to the visible region, but the introduction of deep impurity levels was found to accelerate photogenerated carrier recombination. Fortunately, the rational doping of Mo was found to mitigate this negative effect. Accordingly, Mo, C co-doped TiO 2 was synthesized via a facile low-temperature calcination process, resulting in unique band structure that enhanced the photocatalytic oxidation of NH 3 . Notably, in-situ DRIFTS and DFT results demonstrated that the gradual reaction of NH 3 adsorbed on Mo atoms with oxygen species through the N 2 H 4 mechanism, promoting the formation of N 2 . These findings offer insights into the design of efficient photocatalysts for NH 3 removal under visible light, and present a promising technology for indoor air pollution control.
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Tungsten
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2025
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IF 11.2
Qian Qi-Ling,Zeng Zhen-Yun,Chen Wan-Ting,Cheng Yu,Zhang Jia,Li Chuan-Hua,Qian Guang-Ren
The promoter is very important for effective catalysts, and the relationship among active species, promoter, and support is a hot topic in the field of catalysis. This work aims to investigate the influence of the promoter on the formation of effective active species. For this purpose, V was leached out from V-loaded TiO 2 (V/Ti) step by step, and the loaded V was classified into different species based on their performances in the catalytic oxidation of chlorobenzene. As a result, when V/Ti was co-doped with Mo or W, the chlorobenzene conversion rate was increased from 48.1% to 54.0% (Mo) or 61.0% (W) at 210 °C. The enhancement was attributed to the redistribution of V species. Specifically, 7.8% of V was “Inactive” V on V/Ti. This “Inactive” V was transformed into an “Active” species. At the same time, “Highly-active V” amounts were increased from 86.0% (V 3.3 /Ti) to 88.1% (WV 3.3 /Ti) and 87.1% (MoV 3.3 /Ti). According to the mechanism investigation, when W and Mo coexisted with V during the synthesis, V 3+ was oxidized into V 5+ , which is easily invaded into the TiO 2 , created more strong acidic sites, and activated more active lattice oxygens. These are all in favor of the effective catalytic oxidation of chlorobenzene. The new understanding of the promoter effect will help to produce a more effective catalyst using the same amount of active species. Graphical abstract
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COMPOSITES PART B-ENGINEERING
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2025
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IF 14.2
Bingbing Qiu,Donghui Zhang,Ruiming Fang,Yanfang Wang,Banglong Shen,Junhao Dai,Huaqiang Chu
Electrocatalytic hydrogen production is a green and feasible method for obtaining hydrogen energy. However, the bottlenecks of high cost, low catalytic activity and inferior stability urgently need to be addressed, and constructing advanced catalysts with optimized microscopic morphology and crystal structure is a feasible and effective strategy to overcome this barrier. Herein, an artful strategy of in-situ grown coupled with N doping and C encapsulation was employed to obtain the NC/NiO–Mo/NF with biomimetic cattle stomach-liked porous structure, which can offer shortcut for ion transportation and expose more active sites for H∗ adsorption. Particularly, the constructed NiMoO 4 –NiO heterojunction in NC/NiO–Mo/NF can significantly boost the hydrogen evolution activity. Meanwhile, the density functional theory (DFT) confirm that the construction of the crystalline-amorphous heterojunction induces electron transfer from NiMoO 4 to NiO, promoting a downshift in the d-band center, thereby achieving a near-thermoneutral free energy for the hydrogen evolution reaction (HER). The de-signed electrocatalyst exhibits exceptional HER activity, with a small overpotential of 48 mV to achieve a current density of 10 mA cm −2 . It is important that NC/NiO–Mo/NF exhibits exceptional HER stability, with current density of 50 mA cm −2 for 100 h. The finding provides a feasible strategy for the fabrication of nonprecious-metal-based HER electrocatalysts with high activity and stability toward industrial water electrolysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Wei Wen,Zimei Fu,Man Zhao,Na Gao,Qinyun Yan,Liwu Qiang,Shuai He,Ze Wang,Lifang Shi,He Xiao,Jianfeng Jia
Electrocatalytic urea oxidation reaction (UOR) offers a sustainable route for wastewater remediation and energy-saving hydrogen production, yet its efficiency is hindered by the sluggish kinetics of conventional nickel-based catalysts following an indirect oxidation mechanism. Here, we report a Mo-regulated Ni 2 P-MoO x heterostructure anchored on black phosphorus (BP) nanosheets, synthesized via an innovative electrolysis-solvothermal strategy, which shifts the UOR pathway from indirect to direct oxidation. Unlike traditional NiOOH-mediated processes, which require prior Ni 2 + oxidation, the in-situ Raman and LSV results indicate that this catalyst enables urea oxidation at unprecedentedly low potentials (1.31 V vs. RHE at 10 mA cm −2 ) before Ni 2+ self-oxidation, thereby reducing the overpotential by 245 mV relative to oxygen evolution. Advanced in-situ characterizations ( In-situ FTIR, In-situ Raman , In-situ EIS) and electronic structure analyses elucidate that Mo dopants with electron-deficient 4d orbitals synergistically enhance urea adsorption via carbonyl coordination and optimize charge transfer through interfacial electronic coupling with Ni 2 P, while phosphorus modulates the d-band center. This unique configuration promotes the direct dehydrogenation of adsorbed urea by electrophilic OH species, accelerates C–N cleavage, and minimizes harmful byproducts. This Ni 2 P-MoO x /BP catalyst sustains 55 h operation at 50 mA cm −2 , demonstrating exceptional stability. This work establishes a paradigm for steering reaction mechanisms through electronic engineering, offering transformative insights for designing energy-efficient electrocatalysts for complex molecule valorization.
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Journal of the American Chemical Society
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2024
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IF 14.4
Yanliang Zhou,Lili Liang,Congying Wang,Fuxiang Sun,Lirong Zheng,Haifeng Qi,Bin Wang,Xiuyun Wang,Chak-tong Au,Junjie Wang,Lilong Jiang,Hideo Hosono
To date, NH3 synthesis under mild conditions is largely confined to precious Ru catalysts, while nonprecious metal (NPM) catalysts are confronted with the challenge of low catalytic activity due to the inverse relationship between the N2 dissociation barrier and NHx (x = 1–3) desorption energy. Herein, we demonstrate NPM (Co, Ni, and Re)-mediated Mo2CTx MXene (where Tx denotes the OH group) to achieve efficient NH3 synthesis under mild conditions. In particular, the NH3 synthesis rate over Re/Mo2CTx and Ni/Mo2CTx can reach 22.4 and 21.5 mmol g–1 h–1 at 400 °C and 1 MPa, respectively, higher than that of NPM-based catalysts and Cs–Ru/MgO ever reported. Experimental and theoretical studies reveal that Mo4+ over Mo2CTx has a strong ability for N2 activation; thus, the rate-determining step is shifted from conventional N2 dissociation to NH2* formation. NPM is mainly responsible for H2 activation, and the high reactivity of spillover hydrogen and electron transfer from NPM to the N-rich Mo2CTx surface can efficiently facilitate nitrogen hydrogenation and the subsequent desorption of NH3. With the synergistic effect of the dual active sites bridged by H-spillover, the NPM-mediated Mo2CTx catalysts circumvent the major obstacle, making NH3 synthesis under mild conditions efficient.
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MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Yijie Wang,Xudong Wu,Dan Chen,Linqian Hou,Dezhi Yang,Hong Li,Yaling Yang
The rapid and sensitive detection of glyphosate herbicide in agricultural products is urgent need. Herein, we develop a photosensitive Fe 3 O v -Mo/P nanozyme with defect-rich rough surface by the co-precipitation method. In particular, the Fe 3 O v -Mo/P nanozyme with high-percentage oxygen vacancy (OV) defects and rough surface exhibited superior peroxidase (POD)-like activity and kinetics. More intriguingly, Fe 3 O v -Mo/P nanozyme with strong optical absorption in near-infrared (NIR) region showed excellent light-promoted POD-like activity. It was found that the defect-rich rough surface is conducive to the adsorption of glyphosate to inhibit the POD-like activity of Fe 3 O v -Mo/P. Under near-infrared laser irradiation, the inhibitory effect of glyphosate on the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by Fe 3 O v -Mo/P was increased by 2.64 times. A colorimetric platform was developed for the detection of glyphosate with a low detection limit of 0.032 mg L -1 and good selectivity. The method was used to determine the residual glyphosate in coffee, and the recovery efficiency was between 91.20–104.00 %. This work that combines the advantage of defect engineering and NIR provides a strategy for developing high-active nanozyme in pesticide assay.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Xiaonan Xu,Nana Luo,Wan-Hui Wang,Ming Bao,Jiasheng Wang
Fatty acid hydrogenation is an important method for the production of fatty alcohols. The combination of Ni and Mo has been reported to be an effective and low-cost catalyst. However, the effect of Mo doping has yet to be fully understood. Here Ni-MoOx/TiO2 catalysts were prepared via simple impregnation. and the enhancement effects of Mo doping were comprehensively revealed. First, MoOx can attract electrons from Ni, reduce the electron density of Ni to improve the intrinsic activity of Ni, and form a Niδ+-(MoOx)δ− heterojunction to induce H2 heterolytic cleavage to active hydrogen ions. Second, the reduction of MoOx generates oxygen vacancies, which can absorb C═O of the fatty acid and facilitate the reaction progression. Third, a Ni1–xMox solid solution can be formed, which can increase the hydrogen adsorption quantity and accelerate the reaction rate. Finally, the bond strength of Mo–O is found to be the most optimum that can absorb the fatty acids while releasing the alcohols so as to recover the oxygen vacancies and avoid overhydrogenation. Therefore, high activity and selectivity for the hydrogenation of carboxylic acid substrates to alcohols can be obtained. Under significantly milder conditions (155 °C, 3 MPa H2) the catalyst provided a 98% yield of lauryl alcohol from lauric acid hydrogenation with a low activation energy of 40.1 kJ/mol. This work could provide an insightful understanding about the effects of Mo doping to Ni on catalyzing hydrogenation reactions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Yu-Zhen Xu,Yu-Le Wang,Yu-Dong Shan,Song-Hai Wu,Yong Liu,Xu Han
Selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) by O2 under solvent- and initiator-free conditions is a challenge in chemical processes, which is still constrained by its low selectivity (theoretical selectivity of 50.0%). Given the low epoxide selectivity (<20.0%) of single metal catalysts, we propose a relay catalysis strategy on the oxidation of Cy to Cy-ep with high selectivity by the spherical Mg–Mo bimetallic oxide (MMO). Such a relay catalyst exhibits a desirable Cy conversion of 31.0% and a high selectivity of 49.3% toward Cy-ep. Meanwhile, the high stability and reusability of MMO also indicate its potential to be used for industrial scale-ups. A series of characterizations and DFT calculations reveal that the negatively charged lattice oxygen in [MgII–O–II] adsorbs allylic H of Cy to weaken the bond energy of the allylic C–H bond and form Cy•, and then Cy• rapidly traps O2 to give CyOO•, which subsequently abstracts H from allylic C–H of another Cy to form 2-cyclohexene-1-hydroperoxide (Cy-OOH) and Cy•, achieving the propagation cycle. On the other hand, the Mo(VI) site in MMO catalyzes the produced Cy-OOH peroxo, which then oxidizes Cy to Cy-ep and 2-cyclohexene-1-ol. This work provides insight into the relay catalyst for the epoxidation of olefin with O2 with high selectivity under solvent- and initiator-free conditions.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
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IF 11.2
Yi Li,Shan Yu,Yuehan Cao,Yue Huang,Qiaohao Wang,Yuangang Duan,Lina Li,Kaibo Zheng,Ying Zhou
Maximizing ultrafast electron-transfer kinetics in semiconductor is pivotal but challenging for high-efficiency solar-to-energy during the photocatalytic reaction process due to the intrinsic property of photocatalysts with low surface electron density. Herein, a model photocatalyst CdS@Mo is synthesized through a typical hydrothermal method for modulating the ultrafast electron-transfer to enhance the surface electron density. X-ray absorption fine spectra (XAFS) reveal that Mo is coordinated with S atoms to form a Mo-S 6 configuration which is different from common MoS 2 and Mo foil structures. Based on the femtosecond transient absorption spectra (fs-TAS), it is found that the formation of Mo-S 6 configuration contributes to the fast decay of CdS signal and Mo-S 6 signal reactivation, illustrating the ultrafast electron-transfer (∼2.2 ps) from CdS to Mo-S 6 configuration, which achieves the enhanced electron density of photocatalyst surface. Finally, a holistic photocatalytic performance evaluation discloses that the growing of Mo-S 6 configuration obviously improves the photocatalytic hydrogen evolution (PHE) efficiency of CdS from 28.5 to 47.5 mmol g –1 h –1 with a solar-to-hydrogen (STH) efficiency of 0.10 % which is seldomly discussed in the system containing sacrificial agents. This work opens a new path to modulate the surface electron density by tuning the ultrafast electron-transfer for enhancing reaction efficiency in electron-density-dependent systems.
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危险品化学品经营许可证（带存储）