JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Lixia Wang,Rongfei Ye,Panming Jian,Jiangyong Liu
Metal-free catalysts with environmental friendless, cost-competitiveness and less susceptibility to leaching and poisoning over metal-based catalysts, have revolutionized in the catalysis domain. In this respect, we herein report the first application of cheap and abundant pumpkin-derived N -doped porous carbon for the reduction of 2-methyl-4-nitrophenol assisted by NaBH 4 . The obtained catalyst is cost-competitive, efficient and robust, with an attractive mass-normalized rate constant of 4.73 s −1 g −1 and good recycling performance. Systematical analyses demonstrate that the 2-methyl-4-nitrophenol reduction reaction catalyzed by the N -doped carbon proceeds through the Langmuir–Hinshelwood kinetics and the performance enhancement benefits from the strong adsorption and activation of the substrates induced by the electronic modulation in the carbon framework via N -doping. This study opens up new avenues for the high-value use of pumpkin as well as the development of metal-free strategy in more catalytic applications.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
高影响因子
Environmental Science-Nano
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2021
·Vol. 8
·期 9
·2607-2617
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IF 8.131
Zhen Cao,Hao Li,Shuangyu Zhang,Yunxuan Hu,Jiang Xu,Xinhua Xu
The liquid-phase reduction method with NaBH4 as the reductant is the most widely used method for sulfidized nanoscale zero-valent iron (SNZVI) synthesis. However, it is unclear how the reductant amount (e.g., NaBH4/Fe ratio) affects the physicochemical properties (i.e. Fe0 and S content, surface S speciation, and lattice constant of the Fe BCC structure) and reactivity of SNZVI. Herein, we synthesized SNZVI with different NaBH4/Fe ratios to assess how the NaBH4/Fe ratio affects their properties, and how these properties correlated to the reactivity and selectivity. The S/Fe molar ratio in the particles of SNZVI decreased from 0.15 to 0.02 when the NaBH4/Fe ratio increased from 1.5 to 5, respectively; meanwhile, the yield of SNZVI increased from 20% to 97%. The Fe0 content and the surface S2−/S22− molar ratio ([S2−/S22−]surface) increased with the increase of the NaBH4/Fe ratio, which enhanced the electron transfer of SNZVI. The trichloroethylene reactivity increased ∼8.5-fold when the [S2−/S22−]surface of SNZVI increased from 0.85 to 1.62, while the selectivity decreased from 82.8% to 64.4% accordingly, indicating that [S2−/S22−]surface could be an indicator for predicting the reactivity and selectivity of SNZVI. These results indicate that the NaBH4/Fe ratio is a possible reason for the lab-to-lab variability of SNZVI reactivity. A higher NaBH4/Fe ratio was favorable for the TCE dechlorination reaction while a lower NaBH4/Fe ratio could enhance the electron selectivity.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Kai Xu,Ruoyin Luo,Mingen Wu,Yi Xu,Chenggen Li,Ming Yang,Yuan Dong
Amorphous Co-Eu-B nanoclusters confined in mesoporous Al 2 O 3 were fabricated by an impregnation–chemical-reduction route. Their hydrogen-evolution performance during NaBH 4 hydrolysis was benchmarked against Co-B and Eu-modified Co-B analogues. Structure-activity correlations reveal a three-fold synergy. Geometric confinement by the Al 2 O 3 scaffold prevents nanoparticle agglomeration. Mixed-valent Eu 3+ /Eu 2+ injects electrons into Co via concurrent B → Co and Eu → Co pathways, generating an electron-rich Co δ− core. The Eu-Al-O interface markedly increases Lewis-acid site density, facilitating H 2 O polarization and B-H bond cleavage. Owing to this coupling, the optimised Co-Eu-B/Al 2 O 3 catalyst (Eu/Co = 0.17) delivers a peak hydrogen-generation rate of 2987.81 mL min −1 g −1 at 30 °C, lowers the apparent activation energy to 39.21 kJ mol −1 , and retains full activity over five consecutive cycles-outperforming previously reported Co-based systems. The study elucidates, for the first time, how rare-earth dopants and support engineering co-operate through structural, electronic and acid–base regulation, providing a transferable blueprint for low-cost, highly active and durable hydrolysis catalysts suitable for portable fuel cells and distributed hydrogen technologies.
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高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Wanpeng Zhou,Ruyao Feng,Miaolian Ma,Zhixuan Hu,Tao Yao,Maofeng Zhang
Natural flavonoids, including quercetin, rutin, baicalein and puerarin have been employed for the first time as efficient catalysts in the alcoholysis of NaBH 4 . Among them, quercetin demonstrates optimal catalytic performance for this reaction, achieving an HGR value of 26374 mL H 2 g cat −1 min −1 when 0.2 g NaBH 4 is catalyzed by 50 mg quercetin. The catalytic activity of quercetin is unparalleled for methanolysis of NaBH 4 , particularly at low-temperature; notably, a high HGR value of 1948 mL H 2 g cat −1 min −1 is observed even at −25 °C. Furthermore, the activation energy for the NaBH 4 methanolysis catalyzed by quercetin within a low temperature range of −25 to 25 °C has been calculated to be 17.2 kJ mol −1 . Investigates into the reusability and regeneration of quercetin reveal that over 74 % of its catalytic activity is retained after five consecutive uses; additionally, complete recovery of catalytic activity can be achieved through simple acid treatment. Moreover, kinetic studies indicate that the reaction orders of NaBH 4 methanolysis catalyzed by quercetin obey to first-order kinetics concerning all concentrations: NaBH 4 concentration, catalyst dosage, and methanol content. This study establishes a foundation for practical application involving NaBH 4 in hydrogen production under cold climate conditions typical in Polar Regions or during severe winters at northern latitudes.
研究领域:
化学工程
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材料科学
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能源研究
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DOI
高影响因子
CATALYSIS LETTERS
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2021
·Vol. 152
·期 2
·610-618
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IF 3.186
Zhou Junjie,Yan Jiaying,Meng Xu,Chen Weifeng,Guo Jianfeng,Liu Xiang
Abstract It is still a significant challenge to replace noble metal based catalysts by non-noble metal-based, highly efficient and earth-abundant catalysts in the H 2 generation upon hydrolysis of sodium borohydride. Herein, we first design and synthesize the highly selective and heterogeneous Co x W y nanocomposites from ZIF-67 as robust catalysts for H 2 production upon the hydrolysis of sodium borohydride. Among them, the Co 0.45 W 0.55 nanocatalyst exhibits the highest TOF of 1770 mL H2 g cat −1 min −1 (the TOF related to only cobalt nanoparticles 8401 mL H2 g Co −1 min −1 ) over pure ZIF-67 or W nanoparticles and other ones. In addition, the Co 0.45 W 0.55 catalyst has been successfully recycled at least 5 times without any significant activity loss, although the W (VI) has been partly reduced to W (V), W (IV) and W (0) in the hydrolysis of sodium borohydride. This stability is taken into account by the highly active Co species rather than the activity of W itself. Based on the results obtained, we have shown that Co 0.45 W 0.55 nanocomposite can be a potential candidate for the replacement of a noble metal catalyst for H 2 generation. Graphic Abstract
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Nanomaterials
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2022
·Vol. 12
·期 15
·2550
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IF 5.719
Yuqian Yu,Li Kang,Lixian Sun,Fen Xu,Hongge Pan,Zhen Sang,Chenchen Zhang,Xinlei Jia,Qingli Sui,Yiting Bu,Dan Cai,Yongpeng Xia,Kexiang Zhang,Bin Li
Sodium borohydride (NaBH4), with a high theoretical hydrogen content (10.8 wt%) and safe characteristics, has been widely employed to produce hydrogen based on hydrolysis reactions. In this work, a porous titanium oxide cage (PTOC) has been synthesized by a one-step hydrothermal method using NH2-MIL-125 as the template and L-alanine as the coordination agent. Due to the evenly distributed PtNi alloy particles with more catalytically active sites, and the synergistic effect between the PTOC and PtNi alloy particles, the PtNi/PTOC catalyst presents a high hydrogen generation rate (10,164.3 mL∙min−1∙g−1) and low activation energy (28.7 kJ∙mol−1). Furthermore, the robust porous structure of PTOC effectively suppresses the agglomeration issue; thus, the PtNi/PTOC catalyst retains 87.8% of the initial catalytic activity after eight cycles. These results indicate that the PtNi/PTOC catalyst has broad applications for the hydrolysis of borohydride.Keywords:hydrogen generation;porous titanium oxide cage;PtNi nanoparticles;sodium borohydride hydrolysis
研究领域:
材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Tianyu Tai,Huazhen Cao,Wenyu Feng,Zedong Yin,Huibin Zhang,Guoqu Zheng
NaBH 4 is a promising hydrogen storage material, while faced with enormous difficulties for scale-up application due to regeneration issues. In this study, a highly efficient and economical strategy for the electrosynthesis of NaBH 4 from hydrolysis by-product NaB(OH) 4 has been proposed. By fabricating solid-phase electrodes with NaB(OH) 4 and electrocatalyst etc., the mass transfer process of B(OH) 4 - at the cathode surface was remarkably improved, thus reducing the resistance of the cathodic reaction . Meanwhile, XPS , FTIR , and CV analyses were combined to reveal the reaction path and control steps of B(OH) 4 - reduction to BH 4 − in the electrocatalytic system . The formation of NaBH 4 and intermediates (BH(OH) 3 - , BH 2 (OH) 2 - , and BH 3 (OH) - ) is the gradual replacement of (OH) - in NaB(OH) 4 by H − . Furthermore, this study reveals that PbO has a suitable hydrogen evolution overpotential and excellent selective catalytic activity . The current efficiency for NaBH 4 synthesis via solid-phase electrolysis was up to 68.12 % by systematically regulating various factors.
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高影响因子
Journal of Materials Chemistry A
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2017
·Vol. 5
·期 20
·9723-9732
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IF 8.867
Jiaguang Zheng,Xuezhang Xiao,Liuting Zhang,Shouquan Li,Hongwei Ge,Lixin Chen
A remarkable improvement in the hydrogen desorption performance of Mg(BH4)2–NaBH4 eutectic composite is achieved by simply ball-milling with fluorographene (FG). It is found that the desorption temperature of Mg(BH4)2–NaBH4 (∼200 °C) is still too high and liquid phase appears during dehydrogenation. Particularly, the novel bowl-like 3D Mg(BH4)2–NaBH4–FG composite can be formed after ball-milling. The novel Mg(BH4)2–NaBH4–FG exhibits a low dehydrogenation temperature of 114.9 °C with 6.9 wt% of pure hydrogen in seconds. In-depth investigations show that such greatly improved hydrogen desorption properties of the Mg(BH4)2–NaBH4–FG composite could be ascribed to both the “novel bowl-like 3D structure” with large specific surface area and the “reactant destabilized modification” owing to the decrease of the reaction enthalpy caused by the formation of NaMgF3. This finding provides a facile preparation of complex borohydride composites with low dehydrogenation temperature and fast rate, which accelerates its practical application in fuel cells.
研究领域:
材料科学
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氢能存储
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纳米技术
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DOI
高影响因子
ACS Applied Nano Materials
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2019
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IF 0
Tiange Ma,Yunfeng Qiu,Yuanyuan Zhang,Xinyang Ji,Ping-An Hu
The search for efficient overall water-splitting electrocatalysts plays an important role for low-cost hydrogen production. Metal phosphides are promising for integrating hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) properties in one bifunctional electrode, but several challenges still exist and need to be solved. We report a free-standing carbon cloth electrode consisting of iron (Fe)-doped Ni5P4 nanosheet arrays via a hydrothermal reaction and subsequent phosphorization, which effectively drives both HER and OER in the base. The as-prepared Fe-doped Ni5P4 with ultralow Fe conent (2.5 atom %) delivers a current density of 10 mA cm–2 at 131 mV for HER and needs 257 mV to reach a current density of 100 mA cm–2 for OER. Overall, water splitting requires only 1.50 V to reach a current density of 10 mA cm–2. The introduction of trace Fe in Ni5P4 is effective to modulate the adsorption energy of the key intermediates for both HER and OER, which is promising for the rational design of transition-metal phosphides based on bifunctional water-splitting catalysts with high performance. In particular, Fe-doped Ni5P4 could effectively catalyze the hydrolysis of NaBH4 with a hydrogen generation rate of 0.175 L g–1 min–1 and an activation energy of 53.41 kJ mol–1, comparable to most transition-metal-based electrocatalysts.
研究领域:
电催化
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氢能
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材料科学
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纳米材料
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能量转换
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DOI
Journal of Environmental Chemical Engineering
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2026
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IF 7.5
Qiaochu Zhou,Yiyang Wang,Zhe Zhang,Chi Zhang,Fang Li,Qiming Li
Hydrogen production from NaBH 4 hydrolysis is a promising approach to on-site H₂ supply, but its practical use is constrained by insufficient catalytic activity and stability of current catalysts. Here Co 3 O 4 catalysts doped with different transition metal ions (W, Ni, Cu and Mo) were prepared via a combined citric-EDTA acid complexation and applied for H 2 generation via NaBH 4 hydrolysis. Effects of various transition metal ions on crystal structure, surface morphologies, and catalytic performance of Co 3 O 4 catalysts were systematically investigated. It can be found that minor doping of transition metal ions does not change the bulk spinel structure of Co 3 O 4 catalysts but can obviously impact its crystallinity and surface morphologies. Moreover, Co 3 O 4 catalysts exhibit distinct induction periods before reaching maximum catalytic activity, with the duration dependent on the type of metal dopants. Notably, Ni-doped Co 3 O 4 catalysts exhibit the highest catalytic activity of 2320 mL·min -1 ·g -1 and a relatively low activation energy of about 25.27 kJ·mol -1 . By contrast, Cu doping exerts a negative effect on the stability of pristine Co 3 O 4 . The catalytic performance follows the order Ni > Mo > W > Cu, with Cu‑doped Co 3 O 4 showing a significantly degraded activity of only 1380.4 mL·min -1 ·g -1 . Meanwhile, an excessively high doping content results in decreased catalytic activity for all samples. This work clarifies the correlation between transition metal doping and Co 3 O 4 optimization, offering theoretical guidance for rational design of high-performance NaBH 4 hydrolysis catalysts.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2025
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IF 5.4
Yisha Zheng,Huiqin Zhang,Qiuwen Huang,Yanhui Zhang,Xian Zhang,Wenlong Xiang
Tetracycline hydrochloride (TCH), as a representative antibiotic pollutant, poses significant environmental risks due to its persistence and ecotoxicity. Conventional degradation technologies are often hampered by inefficiency and high operational costs. To overcome these limitations, a simple sodium borohydride (NaBH 4 ) reduction method was employed to modify CoFe Prussian blue analogue (CoFe-PBA), significantly its intrinsic activity. Subsequently, low-level Cu loading (2 wt%) was introduced, further substantially boosting the degradation efficiency. Comprehensive characterization confirmed that this sequential modification optimizes the material structure and enhances the density of active sites. The optimized 2 %Cu/CoFe PBA catalyst efficiently activated peroxymonosulfate (PMS), achieving >96 % TCH removal within 30 min under optimal conditions. In addition, the 2 %Cu/CoFe PBA exhibited excellent stability across a broad pH range (5–11) and in complex anionic environments. Radical quenching experiments and mechanism analysis revealed that non-radical singlet oxygen ( 1 O 2 ) and sulfate radical (SO 4 · − ) pathways were the dominant contributors to TCH degradation, with superoxide radical (O 2 · − ) and hydroxyl radical (∙OH) playing comparatively minor roles. This high performance stems from synergistic Fe/Co/Cu interactions promoting efficient PMS activation. This work provides a facile, efficient modification strategy (NaBH 4 reduction and minimal Cu loading) for PBAs and clarifies the predominant reactive species responsible for high-performance antibiotic degradation.
研究领域:
环境科学
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催化
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材料科学
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化学工程
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水处理
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Shuqing Zhou,Qiuling Yang,Yi Liu,Lianrui Cheng,Tayirjan Taylor Isimjan,Jianniao Tian,Xiulin Yang
Crafting resilient catalysts that promote H 2 production through the hydrolysis of hydrogen storage materials like sodium borohydride stands paramount for the impending hydrogen economy. In this study, we propose a versatile metal–organic framework (MOF)-assisted approach to systematically explore the impact of electron-metal support interaction (EMSI) of Ru-modified Co-Sm 2 O 3 (Ru/Co-Sm 2 O 3 ) on H 2 evolution from NaBH 4 hydrolysis. Strategic annealing at 800 °C induces cobalt vacancies on the Ru/Co-Sm 2 O 3 surface, optimizing the exposure of active sites and amplifying mass-charge transfer efficiency. Consequently, the defect-enriched Ru/Co-Sm 2 O 3 showcases an impressive hydrogen generation rate (HGR = 0.430 mol min −1 g catalyst −1 ) and outstanding cycling resilience, eclipsing the performance of most contemporary catalysts. Experimental findings reveal that Sm can not only adjust the Ru lattice spacing to accommodate more BH 4 − , but also modulate the Co vacancy concentration, thus bolstering the charge transport and ameliorating the catalyst's electrical conductivity. DFT calculations confirm that the Michaelis-Menten/Eley-Rideal mechanism is more appropriate to explain the hydrolysis of NaBH 4 .
研究领域:
材料科学
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催化化学
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能源化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）