APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Weiguang Fang,Peng Dai,Haibo Hu,Tongtong Jiang,Huaze Dong,Mingzai Wu
Simultaneous acquisition of satisfactory bifunctional activities toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) for single transition metal sulfides is challenging, which greatly restrict their applications as cathode catalysts in the rechargeable Zn-air batteries (ZABs). Herein, Fe 0.96 S/Co 8 FeS 8 nanoparticles co-embedded in 3D porous N, S codoped carbon (Fe 1 Co 1 S x @NSPC) were fabricated with regulated ratio of iron to cobalt. Compared with single iron sulfide catalyst (Fe 0.96 S@NSPC), the obtained Fe 1 Co 1 S x @NSPC exhibits enhanced activities in both ORR and OER , whose half-wave potential and overpotential (at 10 mA cm −2 ) are 0.82 V, 0.39 V. The improved electrocatalytic activities are believed to be from the synergistic effects between the binary sulfides and the N, S co-doping and the 3D porous structures. As expected, the home-made aqueous ZAB based on Fe 1 Co 1 S x @NSPC exhibits a high peak power density (159 mW cm −2 ), large specific capacity (807 mAh g −1 ) and a long-term charge/discharge cycling stability over 378 cycles at about 852 mV. Moreover, the self-made all-solid-state button ZAB based on Fe 1 Co 1 S x @NSPC shows a high peak power density (71 mW cm −2 ) and a well maintained cycle life at about 841 mV over 100 charge/discharge cycles.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
GREEN CHEMISTRY
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2022
·Vol. 24
·期 24
·9721-9733
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IF 11.034
Lin Huang,Xinhao Yu,Lei Huang,Xingtian Zhang,Li Gu,Yongyong Cao,Wei Li,Jing Hu,Xuebo Cao
With the development of the biodiesel industry, the annual production of the byproduct glycerol has increased to a level of nearly millions of tons. Efficient and clean utilization of glycerol is thus urgent and profitable. Direct glycerol fuel cells (DGFCs) capable of selective oxidation of glycerol and co-generation of electricity and high-value added chemicals seem to be the most compelling technique. Unfortunately, selective and durable electrocatalysts for fabricating DGFCs are still not available so far. Herein, ternary Pt–Pd–Ag alloy nanowires (NWs) are designed and synthesized under the direction of the d-band theory. The resulting Pd–Pt–Ag NWs exhibit significant activity towards the glycerol electro-oxidation reaction (GOR) and oxygen reduction reaction (ORR) in an alkaline medium, which outperforms the bimetallic Pt–Ag alloy NWs and the commercial Pt/C benchmark. Moreover, a homemade DGFC based on bifunctional Pd–Pt–Ag NW anode and cathode can achieve a peak power density of 13.7 mW cm−2 under ambient conditions (∼50% enhancement compared to the DGFC based on the Pt/C benchmark) and deliver a record voltage of 1.13 V ever reported in alcohol-feeding fuel cells. Besides the electricity profits, the DGFC concurrently generates value-added formate as a selective product of glycerol oxidization.
研究领域:
电化学
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材料科学
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能源工程
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催化
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DOI
高影响因子
JOURNAL OF MATERIALS RESEARCH
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2023
·Vol. 38
·期 9
·2359-2368
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IF 2.7
Ma Junjie,Liu Hangcheng,Tao Zeyu,Liu Jianfeng,Yuan Binxia,Pan Weiguo,Shi Zhengrong
In order to reveal the relationship between the structure and the electrochemical oxygen reduction reaction (ORR) activity of different double transition metal decorated catalysts, three different double transition metal and N co-doped carbon material cathode catalyst materials (FeCo–NC, FeNi–NC and CoNi–NC) were prepared in this study. The FeCo–NC catalysts synthesised in this study still showed high ORR activity under alkaline conditions, with a half-wave potential of 0.783 V RHE , a mass activity (MA) of 11.36 A/g (0.77 V RHE ) and an ultimate current density of − 4.46 mA cm −2 ; after 30,000 cycles, the half-wave potential only decreased to 99.3% of the initial potential. Meanwhile, we employ MS to establish three different double transition metal and N co-doped graphene catalysts and to calculate and analyse their desorption properties, leading to the FeCo–NC material being the model with the highest ORR activity, which is consistent with the experimental results. Graphical Abstract
研究领域:
电化学
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材料科学
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催化
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jingjing Li,Wei Xia,Yanna Guo,Ruijuan Qi,Xingtao Xu,Dong Jiang,Tao Wang,Yoshiyuki Sugahara,Jianping He,Yusuke Yamauchi
Iron-based single-atom catalysts (Fe-SACs) containing Fe–N 4 active sites have shown immense potential in the oxygen reduction reaction (ORR). However, the limited ability to adsorb O 2 and catalyze subsequent O–O bond breaking on Fe–N 4 sites has hindered their full potential, especially in acidic electrolytes. Here, we present an approach by utilizing a tunable curved surface to enhance the activity of Fe–N 4 active sites, with theoretical calculations, demonstrating that Fe–N 4 sites anchored on low–curvature surfaces (lc-Fe-N 4 ) is favirable for ORR. Experimental results show that the catalyst exhibits excellent catalytic activity and stability for ORR in acidic electrolytes, with a half-wave potential of 0.82 V vs. RHE, approaching that of commercial Pt/C. This work develops an approach for promoting the catalytic activity by anchoring atomically dispersed Fe–N 4 sites, unlocking their potential for extended use in electrocatalytic and energy storage applications.
研究领域:
材料科学
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电化学
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催化
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能源存储
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产品关联
DOI
高影响因子
Journal of Water Process Engineering
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2026
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IF 6.6
Jingrong Li,Song Sun,Xuehui Zhu,Xue Zhang,Hao Shi,Yuanhong Xu
An ORR/EO-Cl system using commercial electrodes achieves efficient disinfection at 5 mA/cm 2 . • Cathodic H 2 O 2 consumes anodic free chlorine to generate 1 O 2 as the dominant bactericide. • The system suppresses chlorate and chlorite formation in real medical wastewater. • Multi-level oxidative damage to membranes, DNA, proteins and lipids causes irreversible inactivation. Electrochemical disinfection of chloride-rich medical wastewater faces an inherent trade-off: killing pathogens efficiently while avoiding toxic chlorate and chlorite formation. Here we show that coupling oxygen reduction at a commercial carbon felt cathode with chlorine evolution at a DSA@Ru/Ir anode breaks this trade-off. At 5 mA/cm 2 , cathodic H 2 O 2 rapidly consumes anodic free chlorine, generating singlet oxygen ( 1 O 2 ) as the dominant bactericidal species while suppressing chlorate and chlorite. In real hospital wastewater, chlorate drops from 0.66 to 0.39 mg/L, and the system inactivates 10 7 CFU/mL Escherichia coli in 5 min and Staphylococcus aureus in 10 min-using, the energy consumption was 0.1169 kWh/m 3 and 0.2338 kWh /m 3 , respectively. Quenching, flow cytometry, DNA electrophoresis, protein carbonylation and lipid peroxidation collectively confirm that 1 O 2 -driven oxidative stress causes irreversible membrane, DNA, protein and lipid damage. This work offers a low-energy, commercially viable strategy for electrochemical disinfection of real medical wastewater with intrinsic byproduct suppression. Download: Download high-res image (85KB) Download: Download full-size image
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高影响因子
Small
·
2024
·
IF 13
Lian-Hua Xu,Qichang Wang,Liangdong Hu,Dekui Shen,Sheng Chu,Huiyan Zhang
The electrochemical reduction of oxygen is pivotal for advancing emerging energy technologies. Precise control over morphology and electronic structure is essential for enhancing catalytic activity and stability in the oxygen reduction reaction (ORR). In this study, a freestanding carbon electrode is developed by in-situ growth of carbon nanotube (CNT)-encapsulated bimetallic CoM (M = Ni, Fe, Mn, Cu) nanoparticles (NPs) within a hierarchical carbonized wood matrix (CoM@NWCC). The hierarchically porous architecture of the electrode promotes efficient mass transfer during the ORR. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) analyses revealed that incorporating metals such as Ni, Fe, Mn, and Cu modulates the electronic structure of Co, specifically adjusting the distance between the d-band center (E d ) and the Fermi level (E F ), thus optimizing ORR kinetics. Among these, CoNi@NWCC, with its asymmetric electronic configuration, achieves an optimal balance between OH * and OOH * adsorption, significantly enhancing catalytic performance. This study demonstrates the potential of band structure engineering to precisely tailor catalyst properties, offering a cost-effective and high-performance solution for zinc-air batteries (ZABs) suitable for large-scale deployment.
研究领域:
材料科学
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能源技术
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
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2024
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IF 6.7
Xiaoting Zhao,Xieraili Maimaitiyiming,Mamutjan Tursun,He Lin
To enhance the large-scale manufacture of zinc-air batteries (ZAB) and direct methanol fuel cells (DMFC), high-performance oxygen reduction reaction (ORR) catalysts must be developed. In this study, corn stalk binder (CS binder) was added to corn stalk (CS), the ratio between the two was adjusted, and the structure and morphology of the carbon material was altered to create a biocarbon substrate material (15 wt% N/C (CS)) with ORR catalytic activity. It had a half-wave potential (E 1/2 ) that was 29 mV greater than the pure carbon substance from CS (0 wt% N/C(CS)). Using Fe and N coordination-Hemin, an iron single-atom catalyst (15 wt% Fe N/C (CS)) was created based on this. Commercial Pt/C catalysts are anticipated to be replaced by the 15 wt% Fe N/C (CS), which demonstrated exceptional peak power density in both DMFC and ZAB cell tests. The catalytic mechanism of 15 wt% Fe N/C (CS) is explained by density functional theory (DFT), whereby the 15 wt% N/C (CS) carbon substrate rich in faulty structures creates space for the effective use of the iron single-atom reactive sites. Furthermore, the Fe N sites reduced the overpotential of ORR, which promoted the adsorption and reduction of oxygen molecules at the active sites.
研究领域:
材料科学
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能源化学
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催化化学
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产品关联
DOI
高影响因子
Nano Research
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2024
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IF 9.5
Gao Li,Song Yang,Xu Xuebing,Li Chang,Hu Chaoquan
In this study, a Mn-modified Pt-based catalyst loaded on nitrogen-doped Ketjen black (Mn-Pt/NKB) is prepared using a simple ethylene glycol reduction method. The size of Pt nanoparticles (NPs) is effectively controlled by doping with Mn and N. With the smallest average particle size of 1.7 nm, Mn-Pt/NKB demonstrates half-wave potentials of 0.890 and 0.688 V in the alkaline and neutral electrolytes, respectively, which are superior to those of commercial platinum on activated carbon (Pt/C). When applied as an air cathode in aluminum-air battery, it exhibits ultra-high power densities of 190 (alkaline) and 26.2 mW·cm −2 (neutral). Moreover, the voltage remains stable after 5 h of discharge. The practical application performance of the Mn-Pt/NKB catalyst in an aluminum-air battery is better than that of commercial Pt/C. Furthermore, the oxygen reduction reaction (ORR) mechanism on surfaces with different particle sizes is analyzed using density functional theory. Oxygen cracking is the major pathway on the surface of the small particles with lower energy consumption of 0.5 eV, while water molecule cleavage is the major pathway on the surface of the large particles with higher energy consumption of 0.97 eV. The lower energy consumption of the oxygen cracking pathway further confirms the ORR mechanism for higher activity on small-sized surfaces. This study provides a direction for the rational design of Pt-based catalysts for ORR and sheds light on the commercial development of aluminum-air batteries.
研究领域:
电化学
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材料科学
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能源存储
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Yan Zhang,HuiYi Pan,Mengru Wang,Xiying Li,Guifeng Lu
Carbon-based composites, especially for heteroatom incorporation including P, S, N, and B, show excellent performance in the ORR and are promising alternatives in place of Pt/C catalysts. However, complex procedures are necessary for the synthesis of the precursors acting as suitable carbon-based electrocatalysts. Herein, a simple method, based on the Schiff-base reaction, offering the privileges of devising the N-containing precursors, is developed to synthesize an efficient ORR catalyst. In this study, a Schiff-base polymer with nanoflower morphology (CNF-P) is synthesized via the reaction of 3,5-diaminobenzoic acid and terephthalaldehyde at room temperature. Subsequently, the N/S-codoped carbonaceous nanoflower electrocatalyst derived from its polymer counterpart (N/S-CNF900) is fabricated through high-temperature pyrolysis of CNF-P with thiourea. Benefitting from the dopants of N and S atoms, the N/S-CNF900 sample demonstrates exceptional ORR activity, offering an E1/2 of 0.87 V, Eonset of 1.02 V, and jm of 6.05 mA cm–2, as well as excellent durability and methanol resistance. When utilized as the air electrode in ZABs, N/S-CNF900 demonstrates superior power output of 178 mW cm–2 coupled with exceptional charge–discharge durability spanning 282 h. The superior electrochemical performance stems from the abundant active sites created by heteroatomic N/S doping with a very high specific surface area and the multilevel porous architecture, thereby ensuring effective exposure of active sites. These findings suggest that the catalyst synthesized through the Schiff-base reaction holds promising potential applications in alkaline zinc–air batteries (ZABs).
研究领域:
材料科学
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电化学
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能源存储
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纳米技术
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高分子化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Runfei Xu,Haoyang Huang,Wenjing Wang,Lei Ding,Qiang Lin,Jinbing Li,Yu Zhang,Yongsheng Han,Jianguo Wang,Xiaohua Lu
We report an approach of direct production of H 2 O 2 from water by applying altering potential in the electrocatalysis. By switching potentials periodically between positive to negative, oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) occurs sequentially on a single electrode loaded catalysts, which leads to the reduction of the newly-formed OER active species, forming H 2 O 2 directly. The H 2 O 2 production is dependent on the time and potentials of OER and ORR, which is optimized in this study. Besides, a waiting time is set after each period to let H 2 O 2 diffusion from the catalyst surface. Different catalysts are employed to test the feasibility of this approach, including glassy carbon, graphene oxide, nickel particles, nickel foam, and palladium particles. All these catalysts result in the production of H 2 O 2 at various reaction rates. Ni offers the highest H 2 O 2 productivity. With the prolonging of the reaction time, the decomposition of H 2 O 2 occurs on the surface of Ni catalysts, which is inhibited by the addition of Zn into the catalysts. The in-situ generated H 2 O 2 is used for partial oxidation of propylene by passing propylene into the porous electrode during the reaction, which lead to the formation of dimethyl ether and adipic acid. This study shows a new route of the direct synthesis and utilization of H 2 O 2 for the generation of valuable chemicals.
研究领域:
电化学
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催化
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化工
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材料科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2017
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IF 5.951
Ling-Xia Zuo,Wen-Jing Wang,Rong-Bin Song,Jing-Jing Lv,Li-Ping Jiang,Jun-Jie Zhu
The demand on the highly efficient and low-cost cathodic electrocatalysts for commercialization of fuel cells is rapidly increasing. One smart route for obtaining these ideal electrocatalysts is extracting active carbon materials from natural and cheap biomass waste. Here, we prepared a novel nitrogen self-doped porous graphitic carbon nanosheets (NPGCNs-NaCl) derived from a nitrogen-rich pruning of Lycium barbarum L. using NaCl crystal as intercalation agent. The as-obtained NPGCNs-NaCl possessed porous structure, large surface area, increased content of nitrogen and high graphitic carbon, and thus making it with high electrocatalytic activity for oxygen reduction reaction (ORR). Most importantly, significantly enhanced stability and tolerance against methanol were observed compared with commercial Pt/C catalyst in alkaline solution. This work is believed to open a new avenue for manufacturing advanced and low-cost ORR electrocatalysts in fuel cells from biomass waste.
研究领域:
材料科学
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电化学
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能源材料
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可持续化学
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Qikai Huang,Xiongwei Zhong,Qi Zhang,Xin Wu,Miaolun Jiao,Biao Chen,Jinzhi Sheng,Guangmin Zhou
Zinc-air batteries (ZABs) with high energy density and safety are promising as next-generation energy storage systems, while their applications are severely hindered by the sluggish reaction kinetic of air cathodes. Developing a bifunctional catalyst with high activity and durability is an effective strategy to address the above challenges. Herein, a Co 3 O 4 /Mn 3 O 4 nanohybrid with heterointerfaces is designed as advanced cathode catalyst for ZABs. Density functional theory calculations show the heterogeneous interface between Co 3 O 4 /Mn 3 O 4 can improve the dynamics of carrier transport and thus enhancing the catalytic activity and durability. The Co 3 O 4 /Mn 3 O 4 catalyst anchored on reduced graphene oxide (rGO) exhibits high oxygen reduction reaction (ORR) activity with a half-wave potential of 0.86 V, and excellent oxygen evolution reaction (OER) activity with the potential of 1.59 V at 10 mA cm −2 , which are comparable to the commercial noble metal catalysts. The improved ORR/OER catalytic activity is ascribed to the synergistic effect of heterointerfaces between Co 3 O 4 and Mn 3 O 4 as well as the improved conductivity and contact area of oxygen/catalysts/electrolytes three-phase interface by rGO. Furthermore, a home-made ZAB based on Co 3 O 4 /Mn 3 O 4 /rGO shows a high open circuit voltage of 1.54 V, a large power density of 194.6 mW cm −2 and good long-term cycling stability of nearly 400 h at 5 mA cm −2 , which affords a promising bifunctional oxygen catalyst for rechargeable ZABs.
研究领域:
材料科学
·
电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子