Catalysts
·
2024
·Vol. 14
·期 3
·205
·
IF 3.8
Pengfei Sha,Xiao Yong,Di Chen,Xing Chen,Fengying Yan,Beili Pang,Hongzhou Dong,Jianhua Yu,Liyan Yu,Lifeng Dong
A Zn–air battery serves as an energy storage solution to address fossil energy and environmental concerns. However, sluggish kinetics in oxygen reduction reactions (ORRs) and oxygen evolution reactions (OERs) demand innovative, cost-effective, and stable bifunctional catalysts to replace precious metal catalysts. In this study, an FeCo-CNTs/KB catalyst was synthesized by pyrolyzing NH2-MIL-101(Fe) coated with glu-Co and conductive carbon (KB). This hierarchical structure comprises carbon nanotubes (CNTs) grafted onto a carbon matrix, housing abundant FeCo nanoparticles within the nanotubes or matrix. KB introduction enhances FeCo nanoparticle dispersion and fosters uniform CNT formation with smaller diameters, thus exposing active sites. Consequently, the FeCo-CNTs/KB catalyst exhibits remarkable bifunctional electrocatalytic activity: an ORR half-wave potential of 0.84 V and an OER overpotential of 0.45 V (10 mA cm−2). Furthermore, the FeCo-CNTs/KB catalyst in a secondary Zn–air battery showcases enduring charge–discharge performance (≥300 h).
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 16
·5579-5589
·
IF 6.119
Qixiao Gai,Shoutian Ren,Xiaochun Zheng,Wenjun Liu,Quanli Dong
Transition metal co-catalysts exhibit considerable potential in the photocatalytic water splitting process, but their limited activity and poor stability inhibit their extensive application, and therefore effective schemes are required to further enhance their co-catalytic performance. In this article, 2D/2D C3N4/CdS heterogeneous photocatalysts are first synthesized, and then CoNi alloyed NPs are selectively loaded on their CdS nanosheets by a convenient photodeposition method. The CoNi loading amount and Co/Ni ratio are adjusted by the photodeposition time and precursor Co2+/Ni2+ ratio, respectively. Meanwhile, Co–S bonds are formed between CdS and CoNi NPs. Their optimal hydrogen evolution rate can reach up to 2936.65 μmol g−1 h−1, which is higher than that of C3N4/CdS with Co, Ni or Pt as co-catalysts (i.e. 844.59, 2385.96 and 2486.66 μmol g−1 h−1), respectively. The enhanced photocatalytic performance should be due to the following three points: (1) the formation of the 2D/2D C3N4/CdS heterojunction; (2) the optimized Gibbs free energy of the CoNi co-catalysts; (3) the formation of Co–S bonds between CoNi and CdS. Our work provides a cost-effective scheme to exploit stable and efficient photocatalysts.
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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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Carbon Capture Science & Technology
·
2022
·
IF 0
Xinrui Wang,Shanshan Xu,Weiting Yang,Xiaolei Fan,Qinhe Pan,Huanhao Chen
This study presents an investigation of using Co doping strategy to improve the Ni on mesoporous SBA-15 catalyst for promoting catalytic dry reforming of methane (DRM) under non-thermal plasma (NTP) conditions. The work was conducted by following the conventional procedures including pre-/post-reaction characterisation of the relevant catalysts, comparative assessment of various scenarios under the NTP condition and longevity tests. However, we found that the performance enhancement of the NTP system was mainly due to the use of the catalytically inert SBA-15 packing, rather than the variation of metal species on it though the results suggest the possible surface reactions on the metal surfaces. Hence, under the NTP condition, the so-called DRM might be mistaken because (i) the production of H 2 and CO was likely due to the electron-impact dissociation of CO 2 /CH 4 in gas discharge and (ii) surface reactions on a DRM catalyst are rather insignificant. We then carefully analysed and reflected on the findings and proposed further research questions to be shared with the colleagues in the field of NTP catalysis.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Kai Ma,Yao Luo,Jietao Wang,Xu Chang,Tong Liu,Yao Wang,Mingyue Ding
Developing robust fuel electrodes with high catalytic activity and stability under CO/CO 2 atmospheres is critical for reversible solid oxide fuel cells (RSOFCs). Here, we report a novel A-site-deficient perovskite Sr 1.95 Fe 1.5 Mo 0.3 Ni 0.2 F 0.1 O 6-δ (SFMNF) synthesized via electrospinning, combining Ni 2+ (B-site cation) and F - (anion) co-doping to enhance CO 2 electrolysis and syngas oxidation performance. Physicochemical characterization reveals that F-doping lowers the crystallization temperature, increases oxygen vacancy concentration, and strengthens CO 2 chemisorption. Reduction under H 2 induces exsolution of Ni 3 Fe alloy nanoparticles. The SFMNF electrode achieves a current density of 233 mA cm -2 at 1.3 V and 750°C in CO:CO 2 =2:1 atmosphere, with 36.2% higher activity than the pre-reduced state. Electrochemical impedance and distribution of relaxation time analyses identify CO 2 adsorption/dissociation as the rate-limiting step. The cell demonstrates exceptional durability over 50 redox cycles and 85-hour of operation without carbon deposition. This work highlights dual doping as an effective strategy to tailor perovskite properties for efficient CO 2 utilization in RSOFCs.
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INDUSTRIAL CROPS AND PRODUCTS
·
2026
·
IF 6.4
Yufei Lao,Hongju Zeng,Bingshen Wu,Yuzhao Qi,Yinliang Zhang,Chuigen Guo,Liping Li,Jinmei Xu
Turning waste natural wood into high-performance carboned electrode. • Constructing N/P co-doped 3D network carbon skeleton within wood tracheids. • NPCW electrode exhibited a high specific surface and CO 2 capture capacity. • NPCW exhibits excellent CO Faradaic efficiency. • Pyrrolic N serves as the primary active site for CO 2 RR. Electrochemical CO 2 reduction reaction (CO 2 RR) has emerged as a pivotal strategy for mitigating excessive CO 2 emissions and achieving carbon neutrality. Carbonized wood (CW) possesses an intrinsic hierarchical porous structure and mechanical strength, rendering it a promising self-supporting and binder-free electrode material for electroreduction CO 2 . However, the catalytic activity of CW is limited due to its low specific surface area and insufficient active sites. Herein, we propose an innovative pore-construction strategy to prepare N/P co-doped 3D network carbon skeleton electrode (NPCW) by impregnating polyvinyl alcohol (PVA), phytic acid (PA), and urea into wood tracheids derived from waste natural wood. This strategy not only boosts electroreduction of CO 2 to CO, providing a sustainable and renewable carbon source for the chemical industry, but also solves the accumulation issue of waste wood that aligns with the green and sustainable principles. The optimized NPCW exhibits high specific surface area (972.6 m 2 g −1 ) and active site density. As a result, NPCW exhibits a remarkable CO 2 capture capacity (4.3 mmol g −1 ), an excellent CO Faradaic efficiency (FE CO ) of 96.7%, and a CO partial current density of −28.7 mA cm −2 , while retaining an FE CO above 80% after 48 h operation. This study offers a green and sustainable strategy to convert waste wood into high-performance carbon electrodes, offering a scalable paradigm for next-generation sustainable electrocatalysts. Download: Download high-res image (248KB) Download: Download full-size image This study proposes an innovative pore-construction strategy to fabricate an N/P co-doped 3D network carbon skeleton electrode (NPCW) by impregnating polyvinyl alcohol (PVA), phytic acid (PA), and urea into wood tracheids derived from waste natural wood. The optimized NPCW exhibits high specific surface area and excellent CO Faradaic efficiency.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Shibo Zhao,Xinjun Wen,Hongge Jia,Mingyu Zhang,Yanqing Qu,Chengbao Geng
The continuous increase in greenhouse gas emissions is having a significant impact on the global climate system. To address this issue, efforts worldwide are promoting the development of clean energy source, with methane-rich biogas being a primary focus. However, the dilution of biogas with CO₂ significantly reduces its calorific value. Therefore, efficient methane purification and resource utilization are urgently required. This study specifically developed a high-efficiency gas separation membrane suitable for large-scale industrial applications. By precisely separating CO₂ from biogas, it provides crucial technological support for enhancing biogas energy quality and promoting its industrialization. Specifically, using a conventional polyimide membrane (6FDA-APAF) as the template, a series of intrinsically microporous polyimide membranes (PIM-PI membranes) were innovatively synthesized by incorporating fluorene-containing microporous units—Namely, 9,9′-bis(4-aminophenyl)fluorene (FDA) or 9,9′-bis(4-amino-3-fluorophenyl)fluorene (FFDA). Subsequent thermal rearrangement (TR) treatment produced PIM-PI(TR) membranes. Both the introduction of fluorene groups and TR treatment increased the interchain spacing of the membranes, with the thermally rearranged PIM-PI(TR) membranes exhibiting larger d-spacings and broader micropore peaks. The 6FDA-FFDA (PIM-PI membrane) achieved a CO₂ permeability coefficient of 151.87 barrer, which is 9.9 times higher than that of the nonporous conventional polyimide membrane (6FDA-APAF, 15.4 barrer). The 6FDA-APAF/FDA (8,2) TR400 [PIM-PI(TR) membrane], subjected to thermal rearrangement, further increased its CO₂ permeability coefficient to 813.80 barrer, representing a 19-fold improvement over the untreated membrane. Simultaneously, this membrane exhibited a CO₂/CH₄ permeability selectivity factor as high as 39.03, surpassing the 2019 Robeson upper bound. Furthermore, both macro- and micro-characterizations reveal structurally uniform and intact membranes. With superior fabrication quality that lays a solid foundation for industrial applications. These results highlight the promising potential of TR-treated PIM-PI (TR) membranes containing fluorene-based pore-forming units for gas separation. This study also offers essential technical support for the industrial application of polyimide membranes in biogas purification
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 2
·D57
·
IF 3.12
Xinkuai He,Zhengyang Sun,Qingtian Zou,Luye Wu,Jianbing Jiang
The electrochemical behavior of Co(II) reduction and Co nucleation/growth process on glassy carbon (GC) electrode in 1-ethyl-3-methylimidazolium bisulfate ([EMIM]HSO4) ionic liquid (IL) and ethylene glycol (EG) system is investigated. Cyclic voltammetry (CV) measurements indicate that Co(II) reduction occurs by a one-step process, Co(II) to Co(0), and it is an irreversible reaction. The diffusion coefficient of Co(II) is 2.24 × 10−6 cm2 s−1 at 323 K in the system. Chronoamperometry measurements show that the growth/nucleation process of Co on GC electrode in [EMIM]HSO4-EG is a three-dimensional (3D) progressive nucleation at lower overpotentials and instantaneous nucleation at higher overpotentials under diffusion controlled growth process. These effects of electrodepositing potential, current density and temperature on Co coating thickness are also investigated. The Co coatings are observed by energy dispersive spectrometer (EDS), scanning electron microscope (SEM) and X-ray diffractometer (XRD). SEM micrographs confirm that the Co coatings are relatively loose with a fibrous surface morphology. XRD pattern of the prepared coating reveals the characteristic peak of crystalline Co with a preferred orientation direction and the average size of Co grains is 11 nm. The nanocrystalline Co coating exhibits an excellent catalytic activity and stability for hydrogen evolution reaction (HER) in alkaline medium.
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FUEL
·
2022
·
IF 8.035
Xiaofang Zhang,Yuhuan Li,Yang He,Debin Kong,Bern Klein,Shenghua Yin,Hongyu Zhao
Activated carbon plays an important role in the field of wastewater treatment due to its excellent adsorption, but improving the recovery and utilization efficiency of activated carbon is a major challenge for its application. In this study, lignite (LC) and poplar leaves (PL) were used as raw materials to prepare magnetic activated carbon (MAC) by co-pyrolysis and char activation modification. The adsorption performance of the product was studied. The results showed that with different blending ratios of LC and PL, a large amount of alkali metal oxides contained in PL had different promoting effects on the pyrolysis of LC. When the mass ratio of LC to PL in the mixture was 3:2, the experimental value of hydrocarbons in the obtained tar reached 53.00%, which was 7.20% higher than the calculated value. The optimal preparation conditions of MAC were determined. Under the conditions of activation temperature of 700 °C, activation time of 2 h, ZnCl 2 mass fraction of 30%, impregnation liquid–solid ratio of 3:1 and impregnation time of 16 h, the activated carbon exhibits a relatively desirable performance. The obtained products were characterized by VSM, XRD, FT-IR, N 2 adsorption and SEM. As a result, the obtained MAC exhibits a better porous structure and higher specific surface area, and Fe 3 O 4 was observed on the surface of the MAC. The adsorption performance of coking wastewater by MAC was studied. We demonstrate that the prepared MAC could effectively adsorb organic matter in wastewater. After MAC was used to adsorb the coking wastewater for 3 h, the COD concentration in the wastewater decreased from 280 to 60 mg/L, and the MAC could be effectively recovered by magnets after adsorption.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Minmin Wang,Min Li,Yilin Zhao,Naiyou Shi,Hui Zhang,Yuxue Zhao,Yaru Zhang,Haoran Zhang,Wenhong Wang,Kaian Sun,Yuan Pan,Shoujie Liu,Houyu Zhu,Wenyue Guo,Yanpeng Li,Yunqi Liu,Chenguang Liu
The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction (HER) in the entire pH range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames (NCFs) anchored with Co single atoms (SAs) and Co nanoparticles (NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire pH range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N 3 coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H 2 O molecule is easily activated and dissociated on Co NPs, while the generated H* is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H 2 O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Hongchao Li,Zihao Zhao,Jieshu Qian,Bingcai Pan
The catalytic activation of peroxymonosulfate (PMS) is under intensive investigation with potentials as an alternative advanced oxidation process (AOP) in wastewater treatment. Among all catalysts examined, Co(II) exhibits the highest reactivity for the activation of PMS, following the conventional Fenton-like mechanism, in which free radicals (i.e., sulfate radicals and hydroxyl radicals) are reckoned as the reactive species. Herein, we report that the primary reactive species (PRS) is proposed to be a Co(II)–PMS complex (Co(II)–OOSO3–), while free radicals and Co(III) species act as the secondary reactive species (SRS) that play a minor role in the Co(II)/PMS process. This Co(II)–OOSO3– exhibits several intriguing properties including ability to conduct both one-electron-transfer and oxygen-atom-transfer reactions with selected molecules, both nucleophilic and electrophilic in nature, and strongly pH-dependent reactivity. This study provides novel insights into the chemical nature of the Co(II)-catalyzed PMS activation process.
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PubMed
高影响因子
Nano Research
·
2020
·Vol. 14
·期 3
·868-878
·
IF 8.183
Lei Zhao,Tan Yangyang,Zhang Zeyi,Wu Wei,Cheng Niancai,Chen Runzhe,Mu Shichun,Sun Xueliang
The construction and design of highly efficient and inexpensive bifunctional oxygen electrocatalysts substitute for noble-metal-based catalysts is highly desirable for the development of rechargeable Zn-air battery (ZAB). In this work, a bifunctional oxygen electrocatalysts of based on ultrafine CoFe alloy (4-5 nm) dispersed in defects enriched hollow porous Co-N-doped carbons, made by annealing SiO 2 coated zeolitic imidazolate framework-67 (ZIF-67) encapsulated Fe ions. The hollow porous structure not only exposed the active sites inside ZIF-67, but also provided efficient charge and mass transfer. The strong synergetic coupling among high-density CoFe alloys and Co-N x sites in Co, N-doped carbon species ensures high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity. First-principles simulations reveal that the synergistic promotion effect between CoFe alloy and Co-N site effectively reduced the formation energy of from O* to OH*. The optimized CoFe-Co@PNC exhibits outstanding electrocatalytic stability and activity with the overpotential of only 320 mV for OER at 10 mA·cm −2 and the half-wave potential of 0.887 V for ORR, outperforming that of most recent reported bifunctional electrocatalysts. A rechargeable ZAB constructed with CoFe-Co@PNC as the air cathode displays long-term cyclability for over 200 h and high power density (152.8 mW·cm −2 ). Flexible solid-state ZAB with our CoFe-Co@PNC as the air cathode possesses a high open circuit potential (OCP) up to 1.46 V as well as good bending flexibility. This universal structure design provides an attractive and instructive model for the application of nanomaterials derived from MOF in the field of sustainable flexible energy applications device.
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