JOURNAL OF HAZARDOUS MATERIALS
·
2016
·
IF 4.836
Yue Yang,Shengming Xu,Zhen Li,Jianlong Wang,Zhongwei Zhao,Zhenghe Xu
Deoiling process is a key issue for recovering metal values from spent hydrotreating catalysts. The oils can be removed with organic solvents, but the industrialized application of this method is greatly hampered by the high cost and complex processes. Despite the roasting method is simple and low-cost, it generates hardest-to-recycle impurities (CoMoO 4 or NiMoO 4 ) and enormous toxic gases. In this study, a novel and facile approach to remove oils from the spent hydrotreating catalysts is developed. Firstly, surface properties of spent catalysts are characterized to reveal the possibility of oil removal. And then, oils are removed with water solution under the conditions of 90 °C, 0.1 wt% SDS, 2.0 wt% NaOH and 10 ml/g L/S ratio for 4 h. Finally, thermal treatment and leaching tests are carried out to further explore the advantages of oil removal. The results show that no hardest-to-recycle impurity CoMoO 4 is found in XPS spectra of thermally treated samples after deoiling and molybdenum is leached completely with sodium carbonate solution. It means that the proposed deoiling method can not only remove oils simply and without enormous harmful gases generating, but also avoid the generation of detrimental impurity and promote recycling of valuable metals from spent hydrotreating catalysts.
研究领域:
化学工程
·
环境科学
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Zhuohang Min,Qi Liu,Nannan Duan,Pengfei Jiang,Jingwen Yang,Ni Xu,Shouchun Ma,Chuanli Qin
Hydrogen is an ideal safe and clean energy source, which can be produced by the electrocatalytic hydrogen evolution reaction (HER). The high overpotential of HER is one of bottlenecks for practical application, thus efficient and stable electrocatalysts, especially inexpensive electrocatalysts, are being vigorously developed to facilitate the reaction. Herein, we report the rational synthesis of a non-noble transition metal electrocatalyst via combined self-assembly and ion-exchange strategy. Zeolitic Imidazolate Framework-67 (ZIF-67) was in-situ grown on the surface of polypyrrole-derived nitrogen-doped carbon nanotubes (N-CNT) through a self-assembly method and then ZIF-67 was transformed into a CoMo layered double hydroxide (CoMo-LDH) through an ion-exchange reaction. As a result, a nanocomposite with N-CNT as the core and CoMo-LDH as the shell (N-CNT@CoMo-LDH) was successfully synthesized. The optimal N-CNT@CoMo-LDH exhibits excellent HER performance with a low overpotential of 86 mV at 10 mA cm −2 in 1 M KOH, superior to ZIF-67, CoMo-LDH, N-CNT@ZIF-67 and many reported LDH-based electrocatalysts. Additionally, the N-CNT@CoMo-LDH maintains approximately 86% of its initial current density after 24-h continuous test, with an overpotential increase of only 9 mV after 3000 cycles. The improved electrocatalytic HER performance is primarily attributed to the synergistic interaction between Mo 6+ and Co 2+ /Co 3+ , facilitating the formation of active sites, and N-CNT as core to enhance electron transport rates and inhibit the stacking of CoMo-LDH nanosheets, thus exposing more active sites of CoMo-LDH. Furthermore, its HER is confirmed to be the Volmer-Heyrovsky mechanism. This work provides a promising pathway for synthesizing highly efficient and stable electrocatalysts based on inexpensive non-noble metals.
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DOI
高影响因子
RARE METALS
·
2018
·Vol. 38
·期 1
·1-13
·
IF 1.5
Liu Qi,Wang Wen-Qiang,Yang Yue,Liu Xue-Gang,Xu Sheng-Ming
Aluminum recovery is a key issue for the overall recycling of valuable metals from spent catalysts. This paper focuses on the recovery and regeneration of alumina with high additional value from the spent hydrodesulfurization catalyst CoMo/Al 2 O 3 . The results indicate that 98.13% alumina is successfully leached from the treated spent catalysts by an alkaline leaching process under the conditions of 5 mol·L −1 sodium hydroxide, a liquid/solid ratio of 20 ml·g −1 , a temperature of 160 °C and a reaction time of 4 h. In the leaching residue, no difficult leaching compound is found and cobalt and nickel are enriched, both of which are conducive to the subsequent metal recovery step. The reaction order of aluminum leaching is 0.99. This reaction fits well with the interfacial chemical reaction model, and its apparent activation energy is calculated as 45.50 kJ·mol −1 . Subsequently, γ-Al 2 O 3 with a high specific surface area of 278.3 m 2 ·g −1 , a mean size of 2.2 μm and an average pore size of 3.10 nm is then regenerated from the lixivium, indicating its suitability for use as a catalyst carrier. The recovery and regeneration of alumina from spent catalysts can not only significantly contribute to the total recycling of such hazardous spent catalysts but also provide a new approach for the preparation of γ-Al 2 O 3 with a high specific surface area using spent catalysts as the aluminum sources.
研究领域:
化学工程
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材料科学
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环境工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhuolin Cui,Tingting Hu,Shuqing Yang,Yu Yang,Xueyan Liu,Tao Wang,Huizhi Chen,Chunlai Zeng,Ruizheng Liang,Yubin Zhou
Sonodynamic therapy (SDT) has attracted increasing attention owing to its superior tissue penetration compared with other therapies. However, the development of multifunctional sonosensitizers with imaging capability and high production efficiency of reactive oxygen species (ROS) is still a challenge for current sonodynamic cancer therapy. Herein, we report the design and preparation of amorphous 2D Mn-doped CoMo-layered double hydroxide (a-Mn-CoMo-LDH) nanosheets (NSs) through acid etching-induced crystalline-to-amorphous phase transformation as a highly active nano-agent for magnetic resonance imaging (MRI)-guided SDT. The a-Mn-CoMo-LDH NSs exhibit superior ROS production capacity compared with amorphous CoMo-LDH NSs (∼1.3 times) and crystalline Mn-CoMo-LDH NSs (∼3.9 times) under ultrasound (US) irradiation, which is ∼ 9.9 times of the previously reported TiO 2 sonosensitizer. The doped Mn 4+ in the a-Mn-CoMo-LDH NSs can not only decompose H 2 O 2 into O 2 to alleviate the hypoxia level in tumor microenvironment (TME), but also consume glutathione (GSH) to reduce its clearance of ROS, promoting the SDT performance synergistically. Importantly, the GSH consumption can partially reduce the Mn 4+ to Mn 2+ within the tumors, which can serve as an agent for T 1 -weighted MRI, thus endowing the a-Mn-CoMo-LDH NSs with excellent MRI capability. Therefore, the as-prepared a-Mn-CoMo-LDH NSs with polyethylene glycol modification can be used as an efficient nano-agent for MRI-guided SDT, which can effectively achieve apoptosis of cancer cells in vitro and eradication of tumors in vivo under US irradiation.
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高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Guang Yang,Jin Liang,Tian Lei,Yaxi Zhang,Li Zhang
Transition metal phosphides (TMPs) have emerged as promising candidates for the hydrogen evolution reaction (HER) due to their tunable phases and electronic structures. However, the development of bifunctional electrocatalysts that effectively balance HER and oxygen evolution reaction (OER) for overall water splitting presents a significant challenge. In this work, we report a novel cauliflower-like bimetallic phosphide, CoMo-P, synthesized on ZIF-67-derived NiCo layered double hydroxide (LDH) through a formic acid-assisted electrochemical phosphating process. This innovative approach not only enhances catalytic efficiency for both HER and OER but also offers a rapid, environmentally friendly, and straightforward fabrication method. The incorporation of formic acid during the electrodeposition process plays a crucial role in optimizing the catalyst's composition and microstructure. Specifically, formic acid facilitates the reduction rate of hypophosphite and stabilizes charged intermediates, thereby reducing the electrodeposition energy barrier and enhancing phosphating efficiency. As a result, the CoMo-P(NCL)/NF electrode demonstrates exceptional HER performance in alkaline media, achieving overpotentials of 55 mV and 108 mV at current densities of 10 and 50 mA cm ‑ 2 , respectively, significantly outperforming the control sample without formic acid addition (η 10 = 80.4 mV, η 50 = 142 mV). Moreover, the electrode exhibits remarkable OER activity with overpotentials of 273 mV and 310 mV at 10 and 50 mA cm ‑ 2 , respectively. When employed as a bifunctional catalyst for overall water splitting, the CoMo-P(NCL)/NF electrode pair requires a low cell voltage of 1.574 V to achieve a current density of 10 mA cm ‑ 2 , surpassing the performance of numerous reported bifunctional catalysts. This study provides a promising strategy for the rational design and practical application of high-performance bifunctional electrocatalysts in sustainable energy conversion systems.
研究领域:
材料科学
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电化学
·
可再生能源
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DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Shuisen He,Xueman Wang,Chenglong Wen,Yu Fan
A novel (C 11 H 26 N) 2 Co(MoS 4 ) 2 complex was prepared via the n-octyltrimethylammonium bromide-assisted self-assembly of CoMo precursors for the selective hydrodesulfurization (HDS) of thiophene. The complex was generated by the interaction between the negatively charged CoMo compound and the positively charged n-octyltrimethylammonium ions. Then positively charged bimolecular layers were formed owing to van der Waals forces between the C 11 H 26 N + and the complex, and they were anchored on the negatively charged γ-Al 2 O 3 . Compared with CoMoS/γ-Al 2 O 3 catalysts prepared by impregnation, the optimal CoMoN-0.3/γ-Al 2 O 3 catalyst exhibited better performance for selective HDS due to the enhanced Mo dispersion, the close contact between Co and Mo, and the increased amount of CoMoS phases on γ-Al 2 O 3 . Among these catalysts, the optimal CoMoN-0.3/γ-Al 2 O 3 catalyst with the highest concentration of CoMoS phases exhibited the highest HDS reaction rate constant of 6.95 × 10 -6 mol·g −1 ·s −1 and the best selective factor of 26.1 for the selective HDS of thiophene with 1-hexene.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2026
·
IF 15
Zhang Huifeng,Li Mengyang,Wang Tao,Zhu Huifen,Deng Lin,Guo Fulian,Zhang Zhihua,Hu Tingting,Liang Ruizheng,Cao Min,Li Zhangping
Cancer remains a critical global health burden, posing a severe threat to human life. Photo-sonodynamic therapy (PSDT), which combines photodynamic (PDT) and sonodynamic (SDT) modalities, has emerged as a promising strategy to overcome limitations in tissue penetration and therapeutic precision. Despite progress, the broader application of PSDT is hindered by PDT’s potential phototoxicity/limited therapeutic penetration depth and SDT’s thermal/mechanical damage under high ultrasound (US) power, as well as the complex synthesis of sensitizers and their suboptimal reactive oxygen species (ROS) generation. Here, we engineer Mg-doped defect-rich CoMo-LDH (a-CoMgMo-LDH) nanosheets via a doping-etching strategy to address these challenges, enabling on-demand treatment from superficial to deep-seated tumors. This sensitizer exhibits exceptional dual responsiveness to NIR-II light and US. It achieves a relative singlet oxygen quantum yield (1.53) superior to most reported photosensitizers, while its sonodynamic ROS yield surpasses that of commercial TiO 2 by 22.3 times and outperforms most reported sonosensitizers, ranking among the highest reported. After bovine serum albumin (BSA) functionalization, a-CoMgMo-LDH-BSA triggers ROS-driven apoptosis and immunogenic cell death under dual irradiation, effectively suppressing tumor growth and metastasis. By integrating NIR-II-enhanced PDT/SDT into a single-component platform, this work advances precision oncology with deep-tumor targeting and immune modulation, offering a transformative strategy for clinical translation. Graphical Mg-doped defect-rich CoMo-LDH (a-CoMgMo-LDH) nanosystem is engineered through doping-etching strategy as a new photo-sonosensitizer for highly efficient photo-sonodynamic therapy, which exhibits remarkable ROS generation efficiency under NIR-II/US stimulation, achieving a 1 O 2 quantum yield of 1.53 under NIR-II light irradiation and 22.3 times ROS yields that of commercial TiO 2 under US irradiation, respectively. After bovine serum albumin (BSA) modification, a-CoMgMo-LDH-BSA efficiently kills cancer cells and eliminates tumors by inducing dual-modal ROS generation and immunogenic cell death
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高影响因子
FUEL
·
2025
·
IF 7.5
Shunnian Xu,Kuo Tang,Xiao Feng,Hongxu Gong,Gang Wang
Traditional hydrocracking faces challenges such as excessive alkane cracking, poor dealkylation selectivity and oversaturation of polycyclic aromatics (PAHs). This study developed a hydro-deconstruction catalytic system to precisely dissociate saturated and aromatic carbon structures while preserving product integrity. First, Al-modified dendritic mesoporous silica nanospheres (DMSNs- x , x is SiO 2 /Al 2 O 3 ratio) were synthesized as catalytic materials by hydrothermal method. The objective is to endow the material with suitable acidity and open mesoporous structures, enabling high selectivity for dealkylation and minimizing secondary cracking activity. The effects of aluminum doping on properties and precise dissociation performance of catalytic materials were systematically investigated. Increasing aluminum content enhanced acidity and shifted pore morphology from exterior-expanded mesopores to slit-like micropores. DMSNs-50 (0.28 mmol/g B acid, 15.7 nm pores) demonstrated outstanding alkyl positioning dissociation, achieving 68.4 % dodecylbenzene conversion with 86.5 % dealkylation selectivity, yielding 25.5 m% benzene and 26.8 m% C 9 -C 12 alkanes. Optimizing the active components for hydrogenation is essential to ensure moderate hydrogenation performance and maintain PAH structures. The 3 %CoMo-CM catalyst (3 m% MoO 3 , 0.7 m% CoO 2 ) showed optimal controlled hydrogenation, achieving less than 33 % conversion of phenanthrene, over 60 % selectivity of moderate hydrogenation, and more than 85 % retention of the PAH structure. Microstructural analysis of hydrogenation active phases indicates that the optimal sulfidation was about 38 %. At this point, the size and stacking number of formed MoS 2 slabs were 4.1 nm and 1.9 layers. This catalyst demonstrated excellent hydro-deconstruction for mixed hydrocarbons. It achieved 89 % dealkylation selectivity while retaining over 85 % long-chain alkane and 70 % aromatic ring. During reusability testing, the catalyst primarily deactivated due to the loss of B acid sites and the sintering of the hydrogenation active phase. This innovative catalytic system enables molecular-level transformation of petroleum resources, offering novel approaches for their efficient utilization.
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高影响因子
Small
·
2024
·
IF 13
Rong Chen,Tingting Hu,Yu Lu,Shuqing Yang,Min Zhang,Chaoliang Tan,Ruizheng Liang,Yuji Wang
Photodynamic therapy (PDT) is demonstrated to be effective in inducing antitumor immune responses for tumor metastasis treatment. However, tumor hypoxia, inferior tissue penetration of light, and low singlet oxygen ( 1 O 2 ) quantum yield significantly hamper the efficacy of PDT, thus weakening its immune function. Moreover, PDT-mediated neutrophil extracellular traps (NETs) formation can further reduce the therapeutic effectiveness. Herein, the use of defect-rich CoMo-layered double hydroxide (DR-CoMo-LDH) nanosheets as a carrier to load a typical peptidyl arginine deiminase 4 inhibitor, i.e., YW4-03, to construct a multifunctional nanoagent (403@DR-LDH) for PDT/immunotherapy, is reported. Specifically, 403@DR-LDH inherits excellent 1 O 2 generation activity under 1550 nm laser irradiation and improves the half-life of YW4-03. Meanwhile, 403@DR-LDH plus 1550 nm laser irradiation can stimulate immunogenic cell death to promote the maturation of dendric cells and activation/infiltration of T cells and significantly downregulate H3cit protein expression to inhibit NETs formation, synergistically promoting the antitumor metastasis effect. Taken together, 403@DR-LDH can kill cancer cells and inhibit tumor growth/metastasis under 1550 nm laser irradiation. Single-cell analysis indicates that 403@DR-LDH can regulate the ratio of immune cells and immune-related proteins to improve the tumor immune microenvironment, showing strong efficacy to inhibit the tumor growth, metastasis, and recurrence.
研究领域:
癌症研究
·
纳米技术
·
免疫治疗
·
光动力疗法
·
肿瘤生物学
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分子生物学
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生物医学工程
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DOI
PubMed
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2017
·Vol. 33
·期 5
·993-1000
·
IF 0.767
YANG Kun,YAO Qi-Lu,LU Zhang-Hui,KANG Zhi-Bing,CHEN Xiang-Shu
Noble-metal-free CuMo nanoparticles (NPs) without surfactant or support have been facilely prepared using NaBH4 as a reducing agent. The as-prepared CuMo nanocatalysts were characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution
transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) surface area measurements, and used as catalysts for the hydrolysis
of ammonia borane (AB, NH3BH3) at room temperature. The as-synthesized Cu0.9Mo0.1 NPs exhibited a high activity towards the hydrolysis of AB with a turnover frequency (TOF) of 14.9 min-1, a higher value than that reported for Cu catalysts.
Our synthesis is not limited to CuMo NPs alone, but can easily be extended to CuW (3.6 min-1), CuCr (2 min-1), NiMo (55.6 min-1), and CoMo (21.7 min-1) NPs, providing a general approach to Cu-M (M = Mo, W, Cr) and TM-Mo (TM = Cu, Ni, Co) NPs as a
series of novel catalysts for the hydrolysis of AB. The enhanced activity of bimetallic NPs may be attributed to the synergistic effects of the Cu-M NPs induced by the strain and ligand effects.
研究领域:
催化
·
材料科学
·
纳米技术
·
化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）