PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
·
IF 7.926
Yanqing Cong,Lingjie Ye,Shiyi Zhang,Qiuyu Zheng,Yi Zhang,Shi-Wen Lv
Constructing hollow structure is an effective strategy to boost the activity of heterogeneous catalysts in peroxymonosulfate (PMS) activation. Herein, a newly-designed Ni-CoO yolk-shell hollow sphere was first synthesized by a step-by-step method. Interestingly, the etching treatment of NH 3 ·H 2 O endowed Ni-CoO sphere with hollow yolk-shelled structure, which was beneficial for the increase of specific surface area and the full exposure of active sites. The calcination treatment reduced the charge transfer resistance and enhanced the redox ability of Ni-CoO, further improving its catalytic activity . As expected, 93.1% of diclofenac sodium (DCF) could be rapidly degraded within 5 min over developed Ni-CoO-3/PMS system, and removal efficiency of TOC was as high as 73.3%. Significantly, redox couples of Co 3+ /Co 2+ and Ni 3+ /Ni 2+ were responsible for PMS activation based on radical pathways (namely SO 4 •− , OH • and O 2 •− ). As the typical radical pathway, 1 O 2 was also involved in DCF degradation. More importantly, Ni-CoO-3-PMS* complexes mediated the direct electron transfer between DCF and PMS. Furthermore, Ni-CoO-3/PMS system with great stability had excellent practical application prospect in actual wastewater treatment . In short, current work not only offered a high-efficiency catalyst for PMS activation, but also shared some insights into the research on advanced oxidation processes .
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2023
·
IF 3.1
Xiang Shuang,Guo Yong,Liu Xiaohui,Wang Yanqin
The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis reactions. Herein, we create the Au-CoO-O V interface in the 1.0%Au/Co 3 O 4 -Rod-250 catalyst, which could dissociate H 2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-O V surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen (signals of Au—D and O—D vibration) compared with bare CoO (Co 3 O 4 -Rod-250). This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Yuanhui Zuo,Mujia Huang,Wenchao Sheng,Qian Xu,Wenquan Tao,Zhuo Li
To develop high-performance non-precious metal-based electrocatalysts for oxygen reduction reaction (ORR) is an urgent demand. We herein report an ingenious strategy to develop highly selective and competitive precious metal-free ORR electrocatalyst Co/CoO/SnO encapsulated in N-rich mesoporous carbon (CCS@NPC) nanocubes, via a simple one-step introduction of all functional components. Atomically mixed composites with significantly enhanced catalytic activity were obtained by adopting amorphous mesoporous ternary metal oxides CoSnO 3 nanocubes as precursor and template. The synergistic effect of the triphase nanohybrids (Co, CoO & SnO) anchored in nitrogen-doped mesoporous carbon nanocubes promoted the catalytic reactions , owning to the anisotropic morphology, great heterojunction interfaces, and structural stability. The large-scale prepared CCS@NPC exhibited excellent electrocatalytic activity toward ORR with an admirable onset potential (1.01 V) and diffusion-limited current density (5.88 mA cm −2 ). The CCS@NPC showed stronger stability (20 h) and higher methanol tolerance with the concentration up to 8.0 M, compared to that of commercial Pt/C.
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JOURNAL OF MOLECULAR STRUCTURE
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2026
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IF 4.9
Di-Ming Chen,Yu-Ting Shi,Xue-Jing Zhang,Shao-Ming Fang
A robust Al-MOF built from octanuclear [Al 8 (μ 2 -OH) 8 (COO) 12 ] clusters with oxygen-rich 1D channels has been prepared. • It exhibits a high C₂H₆ uptake of 147.6 cm 3 /g and an IAST selectivity of 1.69 for equimolar C 2 H 6 /C 2 H 4 at 298 K and 1 bar. • The separation potential (ΔQ = 1.42 mmol/g) outperforms many reported Al-MOFs, reflecting a balanced capacity–selectivity trade-off. • Combined GCMC, DFT, and MD simulations reveal that multiple C–H···O contacts and greater charge transfer govern the ethane preference. The separation of ethane (C 2 H 6 ) from ethylene (C 2 H 4 ) represents a critically important yet highly challenging process in the petrochemical industry, as these two hydrocarbons possess nearly identical molecular sizes and boiling points. In this work, we report the C 2 H 6 adsorption and separation performance of a three-dimensional aluminum-based metal–organic framework (Al-MOF) constructed from octanuclear aluminum clusters and a tricarboxylate linker, featuring one-dimensional channels decorated with abundant strongly electronegative oxygen atoms originating from coordinated formate groups and μ 3 -OH moieties. The presence of these electron-rich oxygen sites creates a polar pore environment that establishes multiple C–H···O short interactions with C 2 H 6 molecules, thereby imparting a distinct recognition preference toward the paraffin over the olefin. Upon activation, the material exhibits a C 2 H 6 adsorption capacity of 147.6 cm 3 /g at 298 K and 1 bar. The ideal adsorbed solution theory (IAST) selectivity for an C 2 H 6 /C 2 H 4 (10/90) mixture reaches 1.69 at 298 K and 1 bar. Furthermore, the separation potential (Δ Q ), which integrates both adsorption capacity and selectivity, is determined to be 1.42 mmol/g, indicating a well-balanced performance profile. The different adsorption performance of 1a toward C 2 H 6 /C 2 H 4 was thoroughly studied via a combination of GCMC, DFT and MD calculations, which demonstrates that deliberate introduction of electron-rich oxygen functionalities into the pore walls of Al-MOFs represents an effective strategy for enhancing ethane-selective adsorption, positioning the present material as a competitive candidate for energy-efficient ethylene purification. Graphical -Synopsis A robust Al-MOF with octanuclear clusters and oxygen-rich pore walls was synthesized for C 2 H 6 /C 2 H 4 separation. It exhibits preferential C₂H₆ adsorption (147.6 cm 3 /g at 298 K, 1 bar), an IAST selectivity of 1.69 for equimolar mixtures, and a separation potential of 1.42 mmol/g. Combined GCMC, DFT, and MD simulations reveal that stronger C–H···O hydrogen bonding and greater charge difference lead to a more favorable host–guest interaction energy (–1.34 vs. –1.27 eV) for ethane. This work demonstrates that engineering electronegative oxygen sites in Al-MOFs is an effective strategy for energy-efficient ethylene purification. Graphical -Pictogram Download: Download high-res image (322KB) Download: Download full-size image
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DALTON TRANSACTIONS
·
2016
·Vol. 45
·期 15
·6371-6382
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IF 4.177
Fu Yang,Shijian Zhou,Haiqing Wang,Saifu Long,Xianfeng Liu,Yan Kong
Nanospherical hexagonal mesoporous silica (HMS) with a functional mesochannel covered with thin-layer-dispersed cobalt oxide species was directly fabricated via a novel metal-assisted templating method (S0M+I−). In this special method, cobalt ions would be enriched on the surface of the pore wall by physicochemical interactions among the surfactant, cobalt ions and silica. Typically, a metallomicelle template (S0M+) formed from the coordinative assembly of metal cations (Co2+, M+) with neutral surfactant dodecyl amine (DDA, S0) would match with negatively charged silicate oligomers (I−) by counter-ion interactions to assemble into the Co-modified HMS nanosphere. The metallization of DDA micelles and the role of cobalt ions in the assembly process can be demonstrated. Interestingly, the addition of amounts of cobalt apparently affects the size of the HMS nanosphere. Additionally, the coverage of CoO species on the mesochannel is increased with cobalt ions coordinated on the micelles. Finally, the functional Co-HMS with dispersed catalytic active phase and improved structure exhibits a special catalytic activity (yield of ca. 65%) for direct oxidation of phenol to p-benzoquinone with the assistance of a sulfate radical stimulated from cobalt in the presence of peroxymonosulfate.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Ye Pengcheng,Fang Keqing,Wang Haiyan,Wang Yahao,Huang Hao,Mo Chenbin,Ning Jiqiang,Hu Yong
Oxygen evolution reaction (OER) is critical to renewable energy conversion technologies, but the structure-activity relationships and underlying catalytic mechanisms in catalysts are not fully understood. We herein demonstrate a strategy to promote OER with simultaneously achieved lattice oxygen activation and enhanced local electric field by dual doping of cations and anions. Rough arrays of Fe and F co-doped CoO nanoneedles are constructed, and a low overpotential of 277 mV at 500 mA cm −2 is achieved. The dually doped Fe and F could cooperatively tailor the electronic properties of CoO, leading to improved metal-oxygen covalency and stimulated lattice oxygen activation. Particularly, Fe doping induces a synergetic effect of tip enhancement and proximity effect, which effectively concentrates OH − ions, optimizes reaction energy barrier and promotes O 2 desorption. This work demonstrates a conceptual strategy to couple lattice oxygen and local electric field for effective electrocatalytic water oxidation.
研究领域:
材料科学
·
电催化
·
可再生能源
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Tuo Wang,Yifei Cao,Huimin Wu,Chuanqi Feng,Yu Ding,He Mei
In this work, N-Ni 1 Co 3 Mn 0.4 O/NF is synthesized as multifunctional electrocatalyst for hydrogen evolution (HER), urea oxidation reaction (UOR) and hydrazine oxidation reaction (HzOR). The optimal Ni/Co (molar ratio) and the amount of doping Mn are investigated, the sample with Ni/Co = 1:3 and the addition of 0.4 mmol Mn exhibits the best catalytic activity with the largest specific surface area. Then the two-electrode electrolyzers composed of N-Ni 1 Co 3 Mn 0.4 O/NF are constructed, and the results from experiments show that the voltage required for overall hydrazine splitting (OHzS) at 100 mA cm −2 is 0.272 V, 1.614 V lower than that of overall water splitting (OWS, 1.886 V), while the overall urea splitting (OUS) needs 1.669 V, 0.187 V lower than that of OWS, revealing the outstanding thermodynamic and kinetic advantages of OUS and OHzS. The superior performance may be attributed to the heterostructure between metal and metal oxide and N-doping, which can promote electron transfer and optimizes the decomposition of urea and hydrazine hydrate and hydrogen production , and the research on mechanism will be carried out in the future.
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Nanomaterials
·
2021
·Vol. 11
·期 9
·2237
·
IF 5.076
Khalil ur Rehman,Shaista Airam,Xiangyun Lin,Jian Gao,Qiang Guo,Zhipan Zhang
Creating oxygen vacancies and introducing heterostructures are two widely used strategies in Co-based oxides for their efficient electrocatalytic performance, yet both strategies have rarely been used together to design a bifunctional electrocatalyst for an efficient overall water splitting. Herein, we propose a facile strategy to synthesize oxygen-defect-rich Co9S8/CoO hetero-nanoparticles with a nitrogen-doped carbon shell (ODR-Co9S8/CoO/NC) through the in situ conversion of heterojunction along with surface-induced oxygen vacancies, simply via annealing the precursor Co3S4/Co(OH)2/ZIF-67. The as-prepared ODR-Co9S8/CoO/NC shows excellent bifunctional catalytic activities, featuring a low overpotential of 217 mV at 10 mA cm−2in the oxygen evolution reaction (OER) and 160 mV at 10 mA cm−2in the hydrogen evolution reaction (HER). This performance excellency is attributed to unique heterostructure and oxygen defects in Co9S8/CoO nanoparticles, the current work is expected to offer new insights to the design of cost-effective, noble-metal-free electrocatalysts.Keywords:oxygen vacancies;heterojunction;oxygen evolution reaction;hydrogen evolution reaction
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Mingmei Ding,Wang Ao,Hang Xu,Wei Chen,Lin Tao,Zhen Shen,Huihong Liu,Chunhui Lu,Zongli Xie
Photocatalysis and peroxymonosulfate (PMS) based advanced oxidation processes (AOP) are emerging technology for the degradation of refractory organic pollutant in the field of water treatment . Here we report a novel CoO@TiO 2 /MXene (CTM) hybrid through a facile sonication-hydrothermal method for efficient degradation of phenol via an integrated PMS activation-photocatalysis process. Benefiting from the proper position and superior suitability of the band structure, a dual interfacial charge transport channel was constructed, boosting the separation of photo-generated charge carriers and generating sufficient potential difference for redox reaction. Accordingly, the CTM hybrid not only possessed the outstanding photocatalytic activity but also dramatically accelerated PMS activation to generate considerable reactive radicals. As a result, over 96% phenol degradation was achieved in the 10% CTM/PMS/Vis system within 15 min. The radical quenching test and EPR analysis reveal that SO 4 •− , O 2 •− and 1 O 2 were predominant reactive species involved in the catalytic process. Moreover, the damaged chemical structure of CoO during PMS activation could be healed by the photo-actuated Co(II) regeneration to allow for continuous and stable catalytic process. This study offers a promising perspective for the rational design of competent and stable hybrid heterojunction catalyst to construct PMS activation-photocatalysis processes for the efficient degradation of organic contaminants .
研究领域:
环境科学
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材料科学
·
化学工程
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JOURNAL OF POWER SOURCES
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2024
·
IF 8.1
Qihui Ding,Qi Zhang,Binbin Li,Ding Cai,Wei Wu
For rechargeable Zn air batteries (ZABs), the low cost and scalable preparation method for the catalyst with favorable bifunctional oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalytic properties is a critical influence factor for its large-scale application. In this paper, the composites (preTiO 2 @hG) consisting of the precursor of titanium dioxide and hydrophilic graphene were successfully prepared in a Rotating Packed Bed by high-gravity technology. Then, N and Co elements were doped by hydrothermal-reduction method to obtain composite catalyst CoO-TiO 2 @NG, which had excellent catalytic performances of both OER/ORR. The value of ΔE is 0.685 V for CoO-TiO 2 @NG. When used as the catalyst on the air cathode of rechargeable ZABs, the device exhibits a high power density of 146.8 mW/cm 2 and a large specific capacity of 815.8 mAh/g. It also has good cycle stability, the ZAB capacity using CoO-TiO 2 @NG as catalyst does not significantly decrease after more than 110 h of charging-discharging cycles. The improvement of OER and ORR catalytic performance of CoO-TiO 2 @NG is due to the synergistic effect of CoO, TiO 2 and N-doped graphene. This article provides a new method for low-cost and scalable preparation of bifunctional OER/ORR non-precious metal catalysts with novel component and high performances.
研究领域:
材料科学
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电化学
·
能源科学
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Kao Chen,Huailiang Li,Jingyi Chen,Annan Wang,Weiwei Zhu
Highly recoverable and stable heterogeneous catalysts are critical for peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). This work addresses the difficult separation and metal leaching issues of conventional powdered metal–organic frameworks (MOFs) by constructing a self-supporting Co-MOF@chitosan (Co-MOF@CS) composite membrane. Through in situ reconstruction during PMS activation, the low-crystallinity Co-MOF precursor transforms into an amorphous CoO(OH) nanolayer on the membrane surface. The reconstructed active phase anchors firmly on the porous CS substrate, thereby enabling efficient PMS activation by facilitating rapid electron transfer and providing abundant surface active sites. The Co-MOF@CS membrane exhibited excellent catalytic performance, degrading > 96% of the methylene blue (MB) and ∼70% of sulfadiazine (SDZ) after five consecutive cycles. Notably, the degradation efficiency increased slightly after multiple cycles due to continuous exposure of CoO(OH) active sites. The Co species effectively anchored onto the CS matrix through strong coordination, contributing to extremely low cobalt leaching (0.05 to 0.06 mg/L) and outstanding long-term reusability. Radical quenching and electron paramagnetic resonance (EPR) analyses revealed superoxide radicals (O 2 •− ) and singlet oxygen ( 1 O 2 ) as the dominant reactive species. This work elucidates the dynamic self-activation of low-crystallinity Co-MOFs in AOPs while providing a green and sustainable solution to secondary pollution caused by powdered nanocatalysts during water treatment.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Xingyue Wei,Hanmin Zhang,Mengbo Cao
In this study, a series of Co-doped NPC biochar (nCo-NPC) was prepared by one-step pyrolysis of N and P-rich Chlorella pyrenoidosa (CP) waste mixed with cobalt nitrate for heterogeneous catalytic ozonation (HCO) degradation of ibuprofen (IBU). Compared to the HCO process using CoOx or NPC catalysts, the 2Co-NPC catalyst showed superior performance in the degradation of IBU due to the synergistic effect between the CoOx and NPC. The 2Co-NPC catalyst exhibited high stability after five trials, with the removal efficiency decreasing from 99.9 % to 85.4 %. Moreover, hydroxyl radicals ( OH) and adsorbed atomic oxygen (*O) were identified as the main active species in 2Co-NPC HCO process. The coupling of NPC and CoOx formed electron-rich Co(II) center and electron-deficient NPC center. The electron-rich Co(II) center can direct decomposition of adsorbed ozone into *O and further convert to OH. The electron-deficient NPC center gained electrons from organic pollutants, C N, C O, and P groups through C O Co and C N Co bonds, stimulating the π-cation reaction to transfer to the Co(II) center, thus accelerating the cycling between Co(II) and Co(III). Additionally, the deprotonation of surface hydroxyl groups may also serve as a potential active site for the decomposition of ozone into OH. This study used biomass CP as a precursor coupled with cobalt salt, revealing electron transfer pathways and providing new insights for the future developing of low-cost, efficient, and stable ozone catalysts.
研究领域:
环境科学
·
材料科学
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