ELECTROCHIMICA ACTA
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2024
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IF 5.5
Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma
Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.
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ChemistrySelect
·
2025
·Vol. 10
·期 4
·e202405183
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IF 2
Jingwen Zhang,Zeyang He,Hao Fu,Wei Kong,Petr Senin,Arkadii Proskurin,Ting Bian,Shitan Yan
Graphical Phosphomolybdic acid doping and co-etching with thioacetamide at low temperatures resulted in the formation of uniformly Mo-doped CoS₂ nanoparticles exhibiting a hollow structure that increased the number of active sites and provided abundant reaction sites. In terms of performance, Mo-CoS₂ exhibits the competitive OER and HER properties for an efficient overall water splitting. Nowadays, the sluggish hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) kinetics are the key obstacles limiting the commercial application of water splitting. In this study, a size-matching strategy is proposed to construct the molybdenum-doped CoS 2 polyhedra (Mo-CoS 2 ) by encapsulating polyoxometalate (POM, H 3 PMo 12 O 40 ) guests into mesoporous zeolite imidazolium framework-67 (ZIF-67), with thioacetamide (TAA) serving as a gentle sulfur source. The catalyst exhibits a pronounced hollow structure due to the synergistic etching effects of POM and TAA, which can increase the number of active sites. Additionally, the incorporation of Mo optimizes the electronic structure, thereby improving both HER and OER performance. In alkaline electrolytes, Mo-CoS 2 delivers an overpotential of 330 mV and 269 mV for OER and HER, respectively, to produce a current density of 100 mA cm −2 . Moreover, Mo-CoS 2 demonstrates exceptional performance in overall water splitting, achieving a cell voltage of 1.55 V at 10 mA cm −2 , along with outstanding long-term stability. This study provides a promising avenue for the structural and component optimization of cobalt sulfide, which could significantly improve the efficiency of hydrogen production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Luyang Zuo,Rui Li,Qi Liu,Yabing Duan,Hongwei Wang,Huitao Fan,Bo Li,Liya Wang
Solar energy-assisted hydrogen production technology is an essential tool for exploring hydrogen energy. To date, semiconductors have been used as the primary photocatalyst to generate hydrogen via photocatalytic water splitting. However, the high photogenerated electron–hole recombination rate of semiconductor photocatalysts results in a low hydrogen production rate. Herein, the synergistic effect of Mo-ion doping and the incorporation of Ni-based Hofmann-type coordination polymer (Ni–Ni HCP) on the photocatalytic performance of ZnIn 2 S 4 (ZIS) is investigated. The hydrogen production rate of the prepared in-situ Mo doped ZnIn 2 S 4 wrapped Ni-Ni HCP (Ni–Ni HCP/Mo–ZIS) sample under visible-light irradiation is 26.7 mmol g −1 h −1 , which is 10 times that of pure ZIS. Hydrogen production rate test, microscopic characterization, and density functional theory calculation confirm that the proposed dual modulation approach (combined ion doping and heterogeneous structure construction) could effectively increase the photocatalytic efficiency of ZIS. The stability of prepared samples is also examined by four-cycle photocatalytic hydrogen production tests. The proposed integrated method opens a new route for advancing renewable energy technology towards a sustainable future.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yijiang Ge,Qinrui Sun,Hongtao Bai,Jingde Li,Xiaohang Du
Degradation of organic pollutants by in-situ electrochemically synthetic hydrogen peroxide (H 2 O 2 ) in electro-Fenton (EF) system is important for the treatment of wastewater. In this work, a Fe, Mo co-doped N@TiO 2 electrocatalyst was constructed for H 2 O 2 generation and applied to the degradation of organic dyes. The FeMoN@TiO 2 catalyst in 0.1 M KOH exhibits excellent 2e - Oxygen reduction reaction (ORR) activity and stability, with a yield of up to 1409 mmol gcat -1 h −1 and Faraday efficiency (FE) of 83.4 % at −0.7 V (relative to SCE) for more than 10 h. The in situ generated H 2 O 2 delivers benign organic dyes degradation ability with high methylene blue (MB) removal rate of 98.2 % after 2 h in 0.1 M KOH without adding Fe 2+ . After adding Fe 2+ , the EF process occurs to degrade dyes more efficiently, with Congo red and phenol removal rates of more than 99.0 % and Ciprofloxacin (CIP) removal rate of more than 96.0 % in 0.1 M Na 2 SO 4 solution. It is found that Mo doping increases the active sites of the catalyst, while the dopant of Fe can enhance can improve the electron transfer rate between the catalyst and reactants. Additionally, the synergistic Fe and Mo modulate the electronic structure of Ti, increasing the concentrations of Ti 3+ and chemiadsorbed O. This enhances the electronic conductivity and the reactivity of the catalyst, leading to improved ability for H 2 O 2 generation and organic pollutants degradation. Radical quenching experiments show that the in-situ generated H 2 O 2 reacts with added Fe 2+ to produce a large amount of ·OH, which is the main active substance for organic pollutants degradation. This study provides new insights for non-precious metal oxides to replace precious metals towards in-situ production of H 2 O 2 and degradation of pollutants.
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Solar RRL
·
2024
·
IF 6
Xiya Zhao,Zhiyu Li,Xiaochao Zhang,Xiushuai Guan,Changming Zhang,Puqian Tian,Huiqiang Yue,Liyuan Wang,Yadong Bai,Yawen Wang,Song Yang,Caimei Fan
Photo-anode-driven photoelectrocatalytic reduction of CO 2 is an ideal way for solving problems such as the greenhouse effect and environmental crisis. In this study, a one-step hydrothermal method was successfully used for the preparation of BiVO 4 films doped with different mass fractions of Mo. The results show that when Mo was doped at 1.5 wt%, photocurrent densities of up to 4.11 mA·cm -2 were obtained, 3.36 times greater than those of undoped BiVO 4 , and there was a marked cathodic shifting of water oxidation reaction initiation potential. Subsequently, coupling it with the BiOBr nanosheet cathode, the generated CH 3 OH rate reached 45.67 μmol·L -1 ·h -1 ·cm -2 at a low applied voltage of 1.2 V RHE , with a Faraday efficiency of 60.68% for photoelectrocatalytic CO 2 reduction. This work is important for Bi-based thin film self-assembly coupled with photoelectrocatalytic CO 2 systems. This article is protected by copyright. All rights reserved.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jinke Shen,Gege He,Hongyu Mi,Fengjiao Guo,Haiyan Jin,Xiaqing Chang,Shuo Yan,Jieshan Qiu
Although zeolitic imidazolate frameworks (ZIFs) possess the merits of orderly porosity, high permeability, and easy functionalization, the transformation of ZIFs into the real active species and the promotion of the catalytic efficiency and stability are still challenging. Herein, CoMo-based three-dimensional (3D) hollow nanocages composed of interconnected nanosheets are fabricated by in-situ etching metal–organic framework (ZIF-67) under the aid of MoO 4 2− . X-ray photoelectron spectroscopy (XPS) and in-situ Raman confirm that Mo leaching can accelerate surface reconstruction and generate CoOOH active sites after continuous oxidation. Benefiting from the nanostructure and electronic properties after surface reconstruction, the engineered CoMo-30 exhibits the lowest overpotential of 280 mV at 30 mA cm −2 and robust stability over 110 h in 1 M KOH media for oxygen evolution reaction (OER), which significantly surpasses the other counterparts and commercial RuO 2 . Density functional theory (DFT) calculations indicate that CoMo-30 has a lower free energy of *O → *OOH as rate determining step (RDS), suggesting that CoOOH sites play a crucial role in enhancing the activity and kinetics of OER. This work provides valuable insights into the rational design of hollow structures and the structure-composition-activity relationship during the electrochemical reaction process.
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ACS Applied Materials & Interfaces
·
2024
·
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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MICROCHEMICAL JOURNAL
·
2024
·
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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Small
·
2024
·
IF 13
Zhipeng Liu,Jinling Xue,Yibin Fan,Yinshi Li
Rational design of efficient and non-noble metal bifunctional catalysts for alkaline overall water splitting (OWS) electrochemical reactions is of top priority in the development of hydrogen-based energy. Constructing catalysts with unique structures to optimize the intrinsic activity is a promising strategy. In this work, a newly developed Ni 3 Co 3 Mo 100 -BTC-15h catalyst consisting of Ni nanoparticles enriched on the surface along with a core-shell porous structure is prepared via a hydrothermal process. Due to the unique composition and Ni-enriched core–shell structure, the Ni 3 Co 3 Mo 100 -BTC-15h catalyst exhibits enhanced electrocatalytic properties for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in alkaline media. Under the dual tuning and intermetallic phase, the Ni 3 Co 3 Mo 100 -BTC-15h catalyst deliver a lower overpotential of 151 mV and ≈ 136 mV exceeding commercial catalysts for OER and HER. When the Ni 3 Co 3 Mo 100 -BTC-15h is used as bifunctional catalyst for OWS in a two-electrode alkaline electrolyzer, a cell voltage of 1.62 V is required to drive 10 mA·cm −2 comparable to that of commercial Pt/C and RuO 2 catalysts. This work proposes a potential strategy for optimizing the electrocatalytic performance of non-noble metal catalysts for OWS.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Liang Qiao,Qi You,Xinyuan Wu,Huihua Min,Xiaomin Liu,Hui Yang
The Ni-rich Co-poor layered cathode (LiNixCoyMn1–x–yO2, x ≥ 0.9) is a candidate for the next-generation lithium-ion batteries due to its high specific capacity and low cost. However, the inherent structural instability and slow kinetics of Li+ migration hinder their large-scale application. Mo doping is proposed to enhance the crystal structure stability of LiNi0.9Co0.05Mn0.05O2 and to ensure the preservation of the spherical secondary particles after the cycle. The characterization results indicate that Mo doping not only significantly relieves the lattice strain accompanied by H2 → H3 phase transition but also alleviates particle stress accumulation to avoid pulverization. The Mo-modification allows the generation of uniform fine primary particulates and further agglomeration into the smooth secondary particles to inhibit electrolyte penetration. Hence, the Mo-modified sample NCM90-1%Mo displays an excellent capacity retention of 85.9% after 200 cycles at 0.5 C current density, which is 23.8% higher than that of the pristine NCM90. In addition, with the expansion of the Li slab to accelerate Li+ diffusion and the fine primary particles to shorten the Li+ pathway, the NCM90-1%Mo sample exhibits a high discharge capacity of 150 mAh g–1 at 5 C current density. This work provides a new thought for the design and construction of high-capacity cathode materials for the next-generation lithium-ion batteries.
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Molecular Catalysis
·
2024
·
IF 3.9
Weiwen Wang,Mengqi Bian,Hui Zhao,Rui Liu,Qinghai Zhang,Yunlong Qu,Guanghui Chen,Jihai Duan
The direct synthesis of methyl methacrylate from isobutene is of great importance in the chemical industry. The direct oxidation of isobutylene to methacrylic acid is one of the key steps, but the selectivity of methacrylic acid is low in the products of one-step oxidation of isobutylene. The efficient one-step oxidation of isobutylene to methacrylic acid was achieved by preparing a Mo-V-P-Ce/KCsWPAV two-component composite catalyst combining asymmetric lattice oxygen with appropriate acidic heteropolyacid catalysts. The catalyst was characterized using XRD, FT-IR, BET, SEM, and others to analyze its structural properties, dimensional characteristics, and more. Results indicated that the composite catalyst accelerated the crystallization rate, with Ce enhancing the oxidation of the active molybdenum species and promoting oxygen activation to form lattice oxygen, thereby improving the oxidation of isobutylene. The heteropoly acids increased the percentage of medium strong acidic sites, enhancing the selectivity of methacrylic acid. Under optimized conditions, with an atmosphere to isobutylene molar feed ratio of ≥25:1 and a temperature of 400 °C, the Mo-V-P-Ce/KCsWPAV catalyst achieved a remarkable 91 % conversion of isobutylene with a 70 % selectivity towards methacrylic acid. The catalyst shows promise for practical applications in the one-step oxidation of isobutylene to produce methacrylic acid, providing a suitable solution to the problem of isobutylene overcapacity.
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WASTE MANAGEMENT
·
2024
·
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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