INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·Vol. 43
·期 14
·7038-7045
·
IF 4.229
Rui Lu,Min Hu,Caili Xu,Yi Wang,Yun Zhang,Bin Xu,Daojiang Gao,Jian Bi,Guangyin Fan
Developing effective catalysts for hydrogen evolution from hydrolysis of ammonia borane (AB) is of great significance considering the useful applications of hydrogen. Herein, graphitic carbon nitride (g-C 3 N 4 ) prepared through the simply pyrolysis of urea was employed as a support for Rh nanoparticles (NPs) stabilization. The in-situ generated Rh NPs supported on g-C 3 N 4 with an average size of 3.1 nm were investigated as catalysts for hydrogen generation from the hydrolysis of AB under mild conditions. The Rh/g-C 3 N 4 catalyst exhibits a high turnover frequency of 969 mol H 2 · (min·mol Rh ) −1 and a low activation energy of 24.2 kJ/mol. The results of the kinetic studies show that the catalytic hydrolysis of AB over the Rh/g-C 3 N 4 catalyst is a zero-order reaction with the AB concentration and a first-order reaction with the Rh concentration. This work demonstrates that g-C 3 N 4 is a useful support to design and synthesis of effective Rh-based catalyst for hydrogen-based applications.
研究领域:
催化化学
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能源材料
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纳米催化
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氢能源
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反应动力学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 31
·19968-19978
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IF 10.7
Zicheng Huang,Wenjie Shao,Yijuan Zheng,Junyu Wang,Mao Wang,Shuang Li,Xiaohui Xu,Chong Cheng,Changsheng Zhao
Transition metal oxide-based catalysts are known as the most active oxygen evolution reaction (OER) catalysts due to their intrinsic electronic structures and binding strength of oxygenated intermediates. However, even the most active transition metal oxide-based OER catalysts have a turnover frequency far lower than that of the oxygen-evolving complexes in biological systems for intermolecular site aggregation. Herein, we implement the hybridization of a metal–organic framework and tungstic acid (WO3·xH2O-in-MIL-88) to achieve ordered FeNi site isolation at the molecular level and avoid intermolecular decomposition during the catalysis process. The optimized hybrid with 15% tungstic acid (15%-WO3·xH2O-in-MIL-88) achieves a much-enhanced OER activity and stability in terms of a low overpotential of 263 mV to reach a current density of 10 mA cm−2, a low Tafel slope of 39 mV dec−1, and long-term stability, which is much superior to that of the commercial RuO2 catalyst.
研究领域:
材料化学
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电化学
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催化化学
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能源科学
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无机化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 27
·14278-14285
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IF 8.867
Haibo Tang,Xinlong Tian,Junming Luo,Jianhuang Zeng,Yingwei Li,Huiyu Song,Shijun Liao
Transition metal nitrides have recently attracted significant interest as electrocatalysts for the oxygen reduction reaction (ORR) owing to their low electrical resistance and good corrosion resistance. In this paper, we describe the preparation of a Nb-based binary nitride material with a porous nanogrid morphology/structure. The catalyst exhibited good catalytic activity and high stability towards oxygen reduction. We also intensively investigated the effect that doping with a second transition metal had on the performance of the catalyst. We found that the ORR activity of NbN could be enhanced significantly by enriching the d electrons of Nb through doping with a second transition metal, and that doping with cobalt resulted in the best improvement. Our optimal catalyst, Nb0.95Co0.05N, had an ORR activity ∼4.6 times that of NbN (current density @ 0.6 V vs. the RHE). XPS results revealed that Co doping increased the proportion of Nb in a low-valence state, which may be one of the most important reasons for the enhanced performance. Another important reason is the high surface area resulting from the porous nanogrid morphology. As transition metal doping is an attractive way to enhance the activity of nitride catalysts, our work may provide an effective pathway to achieve this.
研究领域:
材料科学
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电化学
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纳米科技
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催化化学
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能源材料
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2017
·
IF 2.299
Yuan-Zi Xu,Cheng-Zong Yuan,Xue-Ping Chen
To design highly efficient and low-cost electrocatalysts for oxygen evolution reaction (OER) is a great challenge for electrochemical water splitting. Here we introduce a simple and cost-effective strategy for one-step synthesis of a three-dimensional Ni 3 S 2 /MoS X (x is close to 3) nanosheets on Ni foam (NF) via a sovelthermal reaction. The electrochemical performance of the Ni 3 S 2 /MoS X nanosheets on NF has been investigated and exhibits superior OER electrocatalytic activity as well as excellent electrochemical durability. As a novel non-noble-metal OER catalyst operating in basic electrolytes, this 3D cathode exhibits an onset overpotential of as low as 165 mV, a Tafel slope of 67.5 mV dec −1 and remarkable long-term stability. This catalyst maintains its catalytic activity for at least 14 h and only affords 50, 100, and 150 mA cm −2 OER current densities at overpotentials of 215 mV, 265 mV and 305 mV respectively.
研究领域:
材料科学
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电化学
·
能源化学
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纳米科技
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催化化学
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 26
·2310387
·
IF 13
Wei Luo,Yanli Yu,Yucheng Wu,Wenbin Wang,Yimin Jiang,Wei Shen,Rongxing He,Wei Su,Ming Li
Rational design of heterostructure catalysts through phase engineering strategy plays a critical role in heightening the electrocatalytic performance of catalysts. Herein, a novel amorphous/crystalline (a/c) heterostructure (a-CoS/Ni 3 S 2 ) is manufactured by a facile hydrothermal sulfurization method. Strikingly, the interface coupling between amorphous phase (a-CoS) and crystalline phase (Ni 3 S 2 ) in a-CoS/Ni 3 S 2 is much stronger than that between crystalline phase (c-CoS) and crystalline phase (Ni 3 S 2 ) in crystalline/crystalline (c/c) heterostructure (c-CoS/Ni 3 S 2 ) as control sample, which makes the meta-stable amorphous structure more stable. Meanwhile, a-CoS/Ni 3 S 2 has more S vacancies (S v ) than c-CoS/Ni 3 S 2 because of the presence of an amorphous phase. Eventually, for the oxygen evolution reaction (OER), the a-CoS/Ni 3 S 2 exhibits a significantly lower overpotential of 192 mV at 10 mA cm −2 compared to the c-CoS/Ni 3 S 2 (242 mV). An exceptionally low cell voltage of 1.51 V is required to achieve a current density of 50 mA cm −2 for overall water splitting in the assembled cell (a-CoS/Ni 3 S 2 || Pt/C). Theoretical calculations reveal that more charges transfer from a-CoS to Ni 3 S 2 in a-CoS/Ni 3 S 2 than in c-CoS/Ni 3 S 2 , which promotes the enhancement of OER activity. This work will bring into play a fabrication strategy of a/c catalysts and the understanding of the catalytic mechanism of a/c heterostructures.
研究领域:
材料科学
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电化学
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催化化学
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纳米材料
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能源材料
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2013
·
IF 3.473
Manhong Liu,Qiang Bai,Hailian Xiao,Yanyan Liu,Jun Zhao,William W. Yu
Colloidal platinum–ruthenium bimetallic nanoparticles with 2.3 nm were synthesized in solution and then immobilized on tin dioxide powder to make a supported nanocatalyst (Pt–Ru/SnO 2 ). The immobilized bimetallic nanoparticles had the same size and size distribution as the solution dispersed ones. Selective hydrogenation of o -chloronitrobenzene to o -chloroaniline was performed over the as-prepared Pt–Ru/SnO 2 nanocatalyst without using any solvent; 99.5% selectivity to o -chloroaniline at ∼100% conversion was achieved.
研究领域:
催化化学
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纳米材料
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有机合成
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绿色化学
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应用化学
✓ 已验证
DOI
高影响因子
Desalination and Water Treatment
·
2024
·
IF 1
Xu Zhang,Fan Yang,Jialing Qin,Huanghu Peng,Zezhou Chen,Lei Che,Shouxin Zhu,Wei Yang
The heterogeneous catalyst of CeO 2 /ZSM5 was applied to hydrolyze Congo red in subcritical water for the first time in the present study. The hydrolysis rate of Congo red could be significantly accelerated by introducing only 5 mg of 5% CeO 2 /ZSM5. The Congo red could be completely hydrolyzed at 220°C for 2 min—a reaction temperature 40°C lower than in the absence of 5% CeO 2 /ZSM5. In addition, the 5% CeO 2 /ZSM5 could be recycled for another run, and its Congo red hydrolysis efficiency and surface morphology showed no obvious change after 3 runs of recycling. The hydrolysis kinetics of Congo red in subcritical water could be well expressed by the Weibull model. The activation energy for hydrolysis of Congo red in subcritical water in the presence of 5% CeO 2 /ZSM5 (104.8 kJ mol –1 ) was much lower than in the absence of 5% CeO 2 /ZSM5 (155.9 kJ mol –1 ). The frequency factors were calculated to be 8.1 × 10 9 and 1.9 × 10 14 min –1 in the presence and absence of 5% CeO 2 /ZSM5, respectively. With these excellent properties, 5% CeO 2 /ZSM5 may prove to be an advantageous catalyst for the hydrolysis of Congo red in textile wastewater, in subcritical water.
研究领域:
环境化学
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催化化学
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水处理技术
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绿色化学
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反应动力学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Qing Cen,Qiaoyuan Gao,Chenlu Zhang,Yingqi Liu,Qi Wang,Qi Wang
In this study, visible-light-active iron tungstosilicate (FeSiW) was fabricated via solvothermal method . Fe 3+ was applied as counter ion to precipitate with silicotungstic acid (H 4 SiW 12 O 40 ) in methanol solution. It can be observed from FT-IR spectra that the Keggin structure of SiW 12 O 40 4− was well maintained in FeSiW. Besides, the effect of different initial molar ratios of Fe 3+ to H 4 SiW 12 O 40 was investigated (from 4:1 to 4:4). By photoelectrochemical characterizations, such as photocurrent response and Mott-Schottky (M-S) plots, easiest generation of electron-hole pairs and lowest charge transfer resistance can be observed on FeSiW with initial molar ratio of 4:3. Moreover, FeSiW with 4:3 ratio also displayed highest activity for photocatalytic reduction of Cr(VI), despite of the largest band gap (ca. 2.71 eV). The lowest unoccupied molecular orbital (LUMO) and highest occupied molecular orbital (HOMO) of the optimized FeSiW were estimated to be +0.03 V and 2.74 V vs NHE, respectively, which were thermodynamically feasible for Cr(VI) reduction and H 2 O oxidation . Even under acidic condition (pH 3), the optimized photocatalyst displayed good stability in cyclic runs. Therefore, the present study opens a new way for heterogeneous polyoxometalates as efficient photocatalyst for environmental application.
研究领域:
环境化学
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材料科学
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光催化
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无机化学
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污染治理
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 151
·期 3
·901-908
·
IF 2.482
Wu Yuting,Yang Long,Wu Bo,Li Jie,Liu Binyao,Ke Gaili,Dong Faqin,Zhou Yong,He Huichao
It has been reported that β -MnO 2 has photocatalytic activity for the oxidative-coupling of 2-naphthols into 1,1′-bi-2-naphthols. Nevertheless, it is hard to exclude the possibility that the oxidative-coupling of 2-naphthols is initiated by β -MnO 2 catalysis in dark due to the insufficient investigations in the related reports. In the present work, the oxidative-coupling of 2-naphthols into 1,1′-bi-2-naphthols with different phases MnO 2 catalysis in dark and under visible-light irradiation were systematically investigated. The results revealed that the oxidative-coupling of 2-naphthols is jointly initiated by MnO 2 catalysis and O 2 -oxidation, not by MnO 2 photocatalysis. Among the α -MnO 2 , β -MnO 2 , γ -MnO 2 and δ -MnO 2 catalysis, β -MnO 2 catalysis has the optimal performance, its selectivity for the oxidative-coupling of 2-naphthols into 1,1′-bi-2-naphthols is close to 100%, and its catalytic capacity could be well retained after multiple using. Our findings provide comprehensive and accurate understanding the catalytic role of MnO 2 for the oxidative-coupling of 2-naphthols into 1,1′-bi-2-naphthols. Graphic In the present work, the oxidative-coupling of 2-naphthols into 1,1′-bi-2-naphthols was proved to be jointly initiated by MnO 2 catalysis and O 2 -oxidation, not by MnO 2 photocatalysis. β -MnO 2 has the optimal catalytic activity for the oxidative-coupling of 2-naphthols relative to α -MnO 2 , γ -MnO 2 and δ -MnO 2 .
研究领域:
催化化学
·
有机合成
·
材料化学
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物理化学
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纳米催化
✓ 已验证
DOI
高影响因子
Advanced Materials Interfaces
·
2018
·Vol. 5
·期 15
·1800515
·
IF 4.834
Lingxia Zheng,Wangwang Hu,Xuwei Shu,Huajun Zheng,Xiaosheng Fang
Cobalt phosphides based materials are considered as promising electrocatalysts for the hydrogen evolution reaction (HER). The catalytic performance can be further enhanced by improving the intrinsic catalytic activity, exposing more active sites and coupling with conductive support. Herein, a novel electrocatalyst based on nitrogen doped reduced graphene oxides decorates with uniformly distributed CoP x nanoparticles with a suitable P/Co ratio ( x = 1.7) via a facile and mild condition. The optimized composite (CoP x /N-rGO) exhibits superior electrocatalytic HER activities with a low overpotential of 104 mV (at 10 mA cm −2 ), a small Tafel slope of 65 mV dec −1 , and long-term stability in the alkaline media, comparable to the performance of other HER electrocatalysts. The remarkable HER performance can be ascribed to the good electrical conductivity of rGO and extra active sites created by nitrogen doping. In addition, the ultrafine nanostructure (average particle size ≈4 nm) and well-dispersed CoP x nanoparticles also help expose more active sites for electrocatalytic reactions, largely hindering the agglomeration and exfoliation. This work provides a versatile route on the design of multifunctional composite materials for renewable energy research with low cost and high activity.
研究领域:
材料科学
·
电化学
·
纳米科技
·
能源化学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Wanlin Qin,Xianliang Li,Yuchi Zhang,Le Han,Zhijin Cheng,Zhijie Li,Yan Xu
The development of electrocatalysts that show multifunctionality towards efficient sensing and energy applications are of great significance. Herein, we report a rational design of photochemical deposition of Ag nanoparticles (Ag NPs) on ZIF-67-decorated carbon nanotube (Ag NPs/ZIF-67 @CNT) hybrid, which exhibits dual-functional capabilities for both effective enzymeless glucose detection and electrocatalytic water oxidation . The distribution of Ag NPs on the ZIF-67-functionalized CNT can be optimized by adjusting the concentration of Ag + aqueous solution during the light illumination process. The optimized Ag NPs/ZIF-67 @CNT composite showed superior glucose-sensing capability with a low determination limit of 0.46 μM (S/N = 3), high sensitivity of 469.4 μA·mM −1 ·cm −2 , wide linearity detection range (0.010–7.0 mM) and short response time (less than 5 s). Also, the Ag NPs/ZIF-67 @CNT composite acting as potential electrocatalyst possessed an overpotential of 286 mV with a Tafel-slope of 80.75 mV dec −1 at 10 mA·cm −2 for high durability water-oxidation reaction. This work provided a feasible way to prepare Ag NPs decorated ZIF-67/CNT with modulated bifunctional catalytic performances via photochemical reduction strategy, which can also provide effective guidance for designing other multifunctional electrocatalysts .
研究领域:
材料科学
·
电化学
·
生物传感
·
能源催化
·
纳米医学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Mingyuan Chen,Yaxin Lv,Peilin Wu,Liuyan Dong,Xingquan He,Lili Cui
To obtain highly active electrocatalyst for the whole electrochemical water splitting is of importance to generate hydrogen. Co(OH) 2 is used as electrocatalyst towards OER, however, the performance can be improved further. Usually, to construct the interface and adjust the electronic environment of electrocatalysts are regarded as powerful ways to improve the activity. Herein, CeO 2 -Co(OH) 2 sheets supported on copper foam (CF) are fabricated by electrodeposition method. The morphology and the electron structure of metals are adjusted by changing the molar ratio of Co to Ce, thus, resulting in different electrocatalytic activity. The optimal hybrids of CeO 2 -Co(OH) 2 exhibits lower overpotentials of 188, 269 mV to reach 10 mA cm −2 towards HER and OER, respectively, and good stability. Notably, it is found that the electroactivity is extremely superior to that of bare CF as well as the counterparts in the literature. Also, we try to employ M(OH) 2 (M = Fe, Ni) to substitute Co(OH) 2 to investigate the effect of species of hydroxides on the electron interaction between CeO 2 and hydroxides, the XPS results indicate that Ce and Co shows stronger electron interaction compared to other two control hydroxides. As electrocatalysts for alkaline full water splitting, CeO 2 -Co(OH) 2 requires a cell voltage of 1.62 V to drive 10 mA cm −2 . Experimental results prove the advantages of the electron engineering and morphology control.
研究领域:
材料科学
·
电化学
·
能源化学
·
纳米材料
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）