Solar RRL
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2024
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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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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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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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Molecular Catalysis
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2025
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IF 4.9
Wei Wang,Rui Zhang,Jiaqing Li,Huai Liu,Wenlong Jia,Junhua Zhang,Dan Li,Lincai Peng
Furans are important scaffolds with applications in pharmaceuticals, polymers synthesis and biofuels. The direct production of new types of furans from glucose is therefore significant but remains a great challenge. Herein, we report a facile strategy to produce acetylfurans directly from glucose over MoCs-SiO 2 , with an increase in yield from 35.8 % to 81.4 % compared with pristine Mo-SiO 2 due to the facilitated C−C bond cleavage of glucose. The incorporation of Cs improved the dispersion of Mo species, induced the formation of partially reduced Mo, increased the Lewis acidity and glucose adsorption of the catalyst, and thus shifting the reaction selectivity from C−C coupling to cleavage. Kinetic studies further demonstrated the positive contribution of Cs as a promoter in lowering the activation energy of C−C bond cleavage. This study provides a promising strategy to broaden the range of furanic compounds derived from glucose for product-oriented biorefineries.
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Small
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2024
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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
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2024
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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
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2024
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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
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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
·
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
·
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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