INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Ruihong Guo,Yujuan Zhang,Xiutang Zhang,Hong Yang,Tuoping Hu
The development of efficient bifunctional catalysts is the key technology to replace oxygen evolution reaction (OER) with hydrazine oxidation reaction (HzOR) with lower theoretical potential to achieve high efficiency and energy-saving hydrogen production . In this work, the Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) composite with flower-like array was prepared by two-step electrodeposition coupled pyrolysis method. The electrochemical measurements showed that the driving voltages of the optimal composite for HzOR and hydrogen evolution reaction (HER) are respectively −118 mV and 47 mV at a current density (j) of 10 mA cm −2 . The excellent performance of Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) composite is attributed to the fact that the flower-like structure exposes more active areas and facilitates the diffusion of electrolyte, the strong electron interaction between Co 0·52 Cu 0·48 /Cu and S –C substrate, which can be verified by X-ray photoelectron spectroscopy (XPS), enhances the electrical conductivity , the Co 0·52 Cu 0·48 /Cu heterogeneous interface reduces the water dissociation barrier and facilitates the dehydrogenation kinetics of N 2 H 4 determined by density functional theory (DFT) calculations. Due to the excellent performance of Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V), the overall hydrazine splitting (OHzS) electrolytic cell was constructed with Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) as electrodes. The results showed the voltages required by the cell are 36, 210 and 282 mV at the current density values of 10, 100 and 200 mA cm −2 respectively, showing that Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) can be used for energy-saving hydrogen production by hydrazine assisted water electrolysis.
研究领域:
材料科学
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电化学
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催化科学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Wei Liu,Xiaoshen Li,Shaohui Xiong,Xueyang Jiang,Jiayan Yan,Xiang Duan,Yingtian Zhang,Qingpeng Cheng,Ye Tian,Xingang Li
CO 2 hydrogenation to methanol is a critical technology for hydrogen energy conversion and a promising approach to mitigate the energy crisis and greenhouse effect. However, developing highly selective catalysts remains a major challenge for its practical application. Herein, we synthesize an efficient CoCuInO-r catalyst with Cu 11 In 9 and Co 0 dual sites on In 2 O 3 via a sol-gel method. The Cu 11 In 9 intermetallic compound enhances H 2 adsorption capacity and strength, and increases oxygen vacancy concentration on the catalyst surface, thereby improving CO 2 activation and hydrogenation efficiency. Meanwhile, Co 0 suppresses the desorption of the *CO species, facilitating its further hydrogenation to methanol. In-situ DRIFTS experiments indicate that the CO 2 hydrogenation to methanol over CoCuInO-r follows the formate pathway. Compared with CuInO-r (containing Cu 11 In 9 on In 2 O 3 ), CoCuInO-r exhibits a ∼20% increase in methanol selectivity and a 2-fold higher methanol space-time yield, reaching 7.68 mmol·g cat -1 ·h -1 at 300 °C and 4 MPa.
研究领域:
催化
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能量转换
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材料科学
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环境科学
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化学工程
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DOI
高影响因子
ACS Catalysis
·
2025
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IF 13.1
Limin Zhang,Huahua Fan,Miao Zhang,Haoqing Zhang,Hao Wang,Bangjian Liu,Jiaxing Zhang,Xiaowa Nie,Guanghui Zhang,Chunshan Song,Xinwen Guo
Cobalt-based catalysts have recently emerged as a promising frontier in propane dehydrogenation (PDH) research. Despite their potential, achieving selective suppression of nonselective metallic cobalt (Co0) species remains a critical challenge. In this work, we report a hollow zeolite architecture (Co@S-1-Hol) that effectively addresses this dilemma through spatial confinement engineering. Through depth-profiling XPS analysis complemented by H2-TPR and UV–vis spectroscopy characterization, we demonstrate a unique cobalt valence distribution where metallic Co0 species are preferentially encapsulated within hollow cavities, while Co2+ ions remain atomically dispersed in the zeolite shell matrix. DFT calculations coupled with kinetic studies reveal that the cavity-confined Co0 clusters serve as the predominant active centers for C–H bond activation. Notably, STEM-EDS mapping and TGA uncover a self-regulating mechanism: the hierarchical hollow structure facilitates rapid and selective coking on nonselective surface sites during initial reaction phases, effectively passivating undesirable side reactions while preserving intrinsic catalytic activity. This spatial engineering strategy endows the Co@S-1-Hol catalyst with superior PDH performance compared to the conventional impregnated Co/S-1 catalyst, exhibiting an enhanced C3H6 formation rate (21.6 mmol gcat–1 h–1, equivalent to 1330 mmol gCo–1 h–1) coupled with a significantly reduced deactivation rate. Under optimized conditions at 550 °C, the catalyst achieves 35% propane conversion with 95% propylene selectivity, representing state-of-the-art performance among reported cobalt-based PDH catalysts. This work not only provides fundamental insights into cobalt active site engineering but also establishes a paradigm for designing spatially modulated zeolite catalysts in alkane dehydrogenation applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Kang An,Siran Zhang,Hong Wang,Ningyan Li,Ziyang Zhang,Yuan Liu
Direct hydrogenation of CO 2 into ethanol has been considered as an up-and-coming way to achieve CO 2 utilization. Ethanol can be generated by reverse water gas shift as well as CO hydrogenation over Co-based catalysts, where the regulation of Co 0 − Co δ+ is critical. Herein, we designed a supported Co-based catalyst doped with gallium, which was derived from Co-Al-O spinel precursor to facilitate synergistic catalyzing for CO 2 -to-ethanol transformation. The selectivity of ethanol reached 20.1 % in a continuous flow fixed micro-reactor over reduced CoGa 1.0 Al 1.0 O 4 /SiO 2 catalyst at 270 °C and 3.0 MPa. Results of characterization show that the existence of the strong interaction between Ga oxide and cobalt induced the configuration of Co 0 − Co δ+ active pairs, which promotes the process of ethanol synthesis by coupling the dissociation (CH x *)/non-dissociation (CO*) of the intermediates. The strategy by tuning the interaction between cobalt and gallium and/or aluminum oxide brings an avenue to tailor Co 0 − Co δ+ active pairs for the hydrogenation of CO and CO 2 .
研究领域:
催化化学
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能源化学
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材料化学
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环境化学
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工业催化
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DOI
高影响因子
FUEL
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2024
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IF 6.7
Yilin Wei,Zhiwei Sun,Qingqing Li,Dan Wu,Jianshe Wang,Yuexing Zhang,Chunbao Charles Xu,Renfeng Nie
Cost-effective and environmentally friendly production of biomass-derived amines under mild conditions is highly desirable but challenging. Herein, bifunctional Co@CoO x catalysts comprised of Co and CoO x were prepared by controllable precipitation-reduction and adopted for furfural (FAL) reductive amination with N 2 H 4 . The structure of Co species can be regulated gradually via tuning reduction temperature, resulting in a significant influence on reductive amination. The optimal CoO x -250 can achieve 96.4 % furfurylamine (FFA) yield at 60 °C, and even 95.8 % at 30 °C. The control experiments and DFT calculations suggest that the metal Co is responsible for H 2 dissociation and C N reduction, while the oxygen-vacant CoO x favors the hydrogen spillover and the C N bond activation, thus resulting in a collaborative effort for FAL reductive amination. The catalyst is stable and versatile for various aldehydes/ketones with amine yields around 95–99 %, showing great potential for industrial application.
研究领域:
催化化学
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生物质转化
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材料科学
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产品关联
DOI
高影响因子
Waste and Biomass Valorization
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2026
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IF 3.1
Huang Yue,Li Lifeng,Ruan Tao,Ouyang Xinping
The catalytic conversion of lignin derivatives into specific chemicals represents a key pathway for achieving high-valued utilization of biomass. A new Ag–Co 0 /Fe 0.04 Co 0.96 O catalyst was constructed for the selective demethoxylation of vanillic acid derived from lignin depolymerization to produce p-Hydroxybenzoic acid. Compared to Ag–Co 0 /CoO, Fe doping suppressed Co reduction, endowing the Ag–Co 0 /Fe 0.04 Co 0.96 O catalyst with suitable hydrogenation activity and more abundant acidic sites. The hydrogen spillover effect inhibited decarboxylation, dehydroxylation, and benzene ring hydrogenation during the demethoxylation reaction. Oxyphilic Fe species changed the adsorption geometry of vanillic acid from parallel adsorption into twist configuration, avoiding the hydrogenation of benzene ring, and thereby improving the demethoxylation selectivity to p-Hydroxybenzoic acid. By optimizing catalyst preparation and reaction conditions to minimize decarboxylation and over-hydrogenation byproducts, the Ag–Co 0 /Fe 0.04 Co 0.96 O catalyst contributed to a 98.52% conversion of vanillic acid and a 89.62% selectivity to p-Hydroxybenzoic acid under 0.4 MPa H 2 , 0.4 MPa CO 2 at 220 °C for 2 h. This research provided a theoretical foundation and practical guidance for the catalytic demethoxylation of phenolic acids, offering new insights into high-valued utilization pathways for biomass. Graphical
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124268
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IF 7.5
Yimin Wang,Jian Li,Xuning Li,Jun Liu,Xiaoqing Liu,Ying Wang,Yongfa Zhang,Guojie Zhang,Yongliang Ma,Junhua Li,Xu Wu
In this study, a non-oxidative regeneration strategy based on regeneration-induced dynamic structural reconstruction in a bimetallic Co–Mn-decorated activated carbon system was developed to address the rapid adsorbent deactivation caused by styrene-derived carbonaceous deposits formed during high-temperature regeneration. Co(NO 3 ) 2 and Mn(NO 3 ) 2 were introduced onto activated carbon (AC) via impregnation, where the mild nitrate etching effect facilitated the high dispersion and stable anchoring of metal species. Structural characterization revealed that the initially coexisting metallic Co 0 and spinel CoMn 2 O 4 undergo progressive structural reconstruction and phase evolution during high-temperature cycling, transforming into a defect-rich Co 0 /CoO/MnO mixed interface , while largely preserving the hierarchical pore structure. The optimized 2.5Co-2.5Mn-AC sample exhibited a high adsorption capacity of 630.8 mg/g along with excellent regeneration stability, retaining 76% of its initial capacity after six adsorption-regeneration cycles at 900 °C under a nitrogen atmosphere. Notably, its cycling performance significantly outperformed pristine AC and monometallic counterparts. The regeneration-induced evolution of Co–Mn interfaces is closely correlated with the generation of oxygen vacancies and enhanced cycling durability. Metallic Co 0 and reduced Co–Mn oxide phases promote the catalytic transformation of styrene-derived species, effectively alleviating irreversible pore blockage and suppressing performance attenuation. Overall, this work proposes a non-oxidative regeneration strategy, offering a generalizable design concept for recyclable carbon-based adsorbents.
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DOI
高影响因子
ACS Catalysis
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2026
·
IF 13.6
Shiwei Wang,Xunxun Li,Yijia Li,Hexin Li,Lei Jing,Zicheng Wen,Yaru Wang,Shouying Huang,Jing Lv,Xinbin Ma
The pursuit of efficient catalysts for methanol oxidative carbonylation to dimethyl carbonate (DMC) is limited by the kinetic challenge of simultaneously activating CO and methanol on conventional single/mixed sites. Here, we demonstrate a Co0–CoOx interfacial engineering strategy via pyrolysis of bimetallic Zn/Co-ZIF to construct Co@NC catalysts. Systematic tuning of Zn/Co ratio and pyrolysis temperature controls nanoparticle size and oxidation state, yielding the optimal catalyst Co@NC-4, which exhibits a high DMC space-time yield (5.9 gDMC g–1 cat. h–1) and selectivity (97.8%). Through DFT and in situ spectroscopic investigations, we reveal a concentration-driven synergistic mechanism: Co0 sites preferentially adsorb and enrich CO, while the adjacent Co0–CoOx interface activates methanol to form methoxy intermediates. The local high CO concentration ensures rapid coupling with methoxy groups at the interface, significantly boosting reaction efficiency. This work establishes a fundamental design principle of spatially resolved bifunctionality for enhanced catalysis in C1 transformations.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Zhi-Rong Fu,Xin Zhang,Jing-Yuan Hao,Yu Han,Yu-Wei Xiang,Bao-Ju Wang,Xiang-Sen Wu,Yong Luo
The Co/NC catalyst for the hydrogenation of adiponitrile (ADN) is of great importance to produce high-value-added hexamethylenediamine (HMDA), which is the raw material for nylon-66. However, current research has not taken the Co particle size distribution effect fully into account for the ADN hydrogenation performance. In this work, Co/NC catalysts with various Co particle sizes using N-doped carbon as the support were prepared to investigate their activity differences. Among all catalysts, the Co/NC catalyst with an average Co particle size of 13.3 nm exhibited the best performance due to its most dispersed Co0 active site, reaching a complete ADN conversion within 40 min with an HMDA selectivity of 83.68%. It displayed a surprising HMDA STY of 49.77 mmol·gcat–1·h–1 under a greatly reduced activation energy (65.30 kJ·mol–1) with a reaction rate constant of 2.98 × 107 min–1. XPS and H2 pulse adsorption characterizations proved that the synergy between the Co0 content and dispersion emerged as the predominant factor governing the catalytic activity. This work provided a promising method for the design of an advanced catalyst for ADN hydrogenation.
研究领域:
催化化学
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化学工程
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材料科学
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有机合成
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产品关联
DOI
高影响因子
ACS Catalysis
·
2015
·
IF 9.312
Zhongzhe Wei,Jing Wang,Shanjun Mao,Diefeng Su,Haiyan Jin,Yihe Wang,Fan Xu,Haoran Li,Yong Wang
The earth-abundant nanohybrids Co0/Co3O4@N-doped carbon nanotubes were fabricated via an efficient thermal condensation of d-glucosamine hydrochloride, melamine, and Co(NO3)2·6H2O. The hybrids furnish excellent catalytic activity and perfect chemoselectivity (>99%) for a wide range of substituted nitroarenes (21 examples) under relatively mild conditions. The high catalytic performance and durability is attributed to the synergistic effects between each component, the unique structure of graphene layers-coated Co0, and the electronic activation of doped nitrogen. Density functional calculations indicate that the inner Co0 core and N species on the carbon shell can significantly decrease the dissociation energies of H2, giving evidence of the ability of carbon shell in the hybrids to enable H2 activation. These results open up an avenue to design more powerful low-cost catalysts for industrial applications.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Fanhui Liao,Weibin Liang,Meixian Li,Donghai Xu,Le Yang
Selective hydrogenation of carboxylic acids to alcohols remains a challenge due to the requirement of synergistic multiple active sites for H2 activation, reactant adsorption, and selective C–O bond scission. Here, we construct a series of Co–Al metal–metal oxide (MMO) catalysts via the hydrogen-induced reduction of layered double hydroxide (LDH) precursors with tunable Co/Al ratios. The optimal Co4Al1-MMO catalyst exhibits highly dispersed Co0 nanoparticles alongside abundant oxygen vacancies (Ov-Co). The Co0/Ov-Co dual sites synergistically promote H2 dissociation and carbonyl oxygen C=O bond activation, while moderate lattice oxygen stabilizes the metastable structure. Under mild conditions (180 °C, 2 MPa of H2, 3 h), the catalyst achieves 100% conversion of octanoic acid with 99% alcohol selectivity, outperforming state-of-the-art noble-metal systems. This work provides a general strategy for engineering cooperative metallic/defective sites in nonprecious MMO catalysts for selective hydrogenation reactions.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ming Chen,Huan Liu,Ying Wang,Zhiyong Zhong,Yu Zeng,Yuxin Jin,Daiqi Ye,Limin Chen
TiO 2 , ZrO 2 and a series of TiO 2 -ZrO 2 (TxZ1, x means the atomic ratio of Ti/Zr = 10, 5, 1, 0.2 and 0.1) composite oxide supports were prepared through co-precipitation, and then 3 wt% Co was loaded through wetness impregnation methods. The obtained 3 wt% Co/TiO 2 (3CT), 3 wt% Co/ZrO 2 (3CZ) and 3 wt% Co/TxZ1 (3CTxZ1) catalysts were evaluated for the oxidative ethane dehydrogenation reaction with CO 2 (CO 2 -ODHE) as a soft oxidant. 3CT1Z1 catalyst exhibits excellent catalytic properties, with C 2 H 4 yield, C 2 H 6 conversion and CO 2 conversion about 24.5 %, 33.8 % and 18.0 % at 650 °C, respectively. X-Ray Diffraction (XRD), in-situ Raman, UV–vis diffuse reflectance spectra (UV–vis DRS), H 2 temperature-programmed reduction (H 2 -TPR), Electron paramagnetic resonance (EPR) and quasi in-situ X-ray Photoelectron Spectroscopy (XPS) have been utilized to thoroughly characterize the investigated catalysts. The results revealed that 3CT1Z1 produced TiZrO 4 solid solution with more metal defect sites and oxygen vacancies (Ov), promoting the formation of Co 2+ -TiZrO 4 structure. Furthermore, the presence of Ov and Ti 3+ can facilitate the high dispersion and stabilization of Co 2+ , as well as suppressing the severe reduction of Co 2+ , leading to superior ethane oxidative dehydrogenation activity. Besides, less Co 0 is beneficial to ODHE reaction, because of its promotion effects for reverse water gas shift reaction ; however, more Co 0 results in dry reforming reaction (DRE). This work will shed new lights for the design and preparation of highly efficient catalysts for ethylene production.
研究领域:
化学工程
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催化
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材料科学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）