MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Ruilin Liu,Xiaoping Wei,Jianping Li
An amperometric method with synergistic electrocatalysis on photoelectrocatalysis was proposed, and it was used for the detection of trace glucose concentrations for the first time. Under illumination of an external xenon lamp light source, the electrocatalytic oxidation reaction of glucose on a Co 3 O 4 -modified electrode produced a synergistic effect on the photoelectrochemical reaction of glucose. The separation of electron–hole pairs generated by the photoelectrochemical reaction was promoted, and the photoelectric conversion efficiency was improved. As a result, the photoelectric current increased, and the sensitivity of the amperometric method was enhanced by about 9 times. The mechanism of synergistic electrocatalysis on photoelectrocatalysis was studied. The method can be used for the determination of glucose with a linear concentration range of 1.0 × 10 −8 M to 3.5 × 10 −7 M. The sensitivity was 7,753 μA cm −2 mM −1 , and the detection limit was 3.6 × 10 −9 M. Compared with conventional photoelectrochemical analysis methods, the chronoamperometric method has higher sensitivity and lower detection limit. The method has been used for the direct determination of trace amounts of glucose in saliva and sweat.
研究领域:
分析化学
·
生物医学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shu Wei Zhang,Mi Zhang,Fang Wang,Han Zeng
Nano-complex consisting of Titanium dioxide and graphene oxide via covalent bonding was proposed to be Laccase immobilization matrix through collaborative effect of chemical tethering and adjacent complexation between TiO 2 and Laccase molecule. Geometrical feature, structural characteristics and physio-chemical properties of nano-composite with Laccase entrapment were systematically characterized and evaluated. Influences of mutual interactions between element of nano-complex and incorporated protein molecule on kinetics of electro-catalysis and efficiency of photo-electrocatalysis for oxygen reduction of Laccase based electrode were quantitatively analyzed. Results from measurements indicated mutual interactions dominated by adjoining ligation would lead to irregular arrangement of protein molecules on the surface of enzyme carrier and decrease the orderliness of nano-complex with Laccase anchoring with improved hydrophilicity. The combination of Laccase with P25 in nano-complex via the static quenching would enhance the utilization efficiency of external illumination with the crippled band gap (Eg) in the indirect mode (∼1.43 eV for nano-composite with Lac integration). Such combination would alter the route of charge transferring which meant the redox site in TiO 2 would play the role of primary electron acceptor and T 1 site in coordination with TiO 2 of integrated Laccase could perform the duty of intra-molecular electron mediator (apparent heterogeneous electron shuttle rate: 2.6 × 10 −3 s −1 ). Electro-catalytic performance on oxygen reduction for Laccase based electrode was limited by the step of substrate diffusion (in the form of free state and entrapment into nano-complex: 2.9 × 10 −4 and 1.8 × 10 −6 s −1 , respectively). As-prepared Lac case based electrode displayed favorable sensing performance to its substrate-dissolved oxygen: high affinity (K M : 46.4 μmol•L −1 ), moderate detection limit (0.34 μmol•L −1 ) and enhanced sensitivity (0.021 μA•L•μmol −1 ).
研究领域:
生物化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
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2022
·
IF 5.304
Xiao Bai,Hang Yin,Chongchao Zhang,Ziyin Yang
Cobalt (Co) based nanomaterials are widely used to construct glucose enzyme-free electrochemical sensors. However, the correlation between anion species and the electrocatalytic activity of Co based nanomaterials remains unproven. In this paper, Co 3 X 4 with different anions (X = O, S, Se) were synthesized for electrochemical sensing of glucose. Co 3 X 4 was characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectrometry (EDX), powder X-ray diffractometry (XRD), and electrochemical techniques. The results showed that anion substitution had a significant effect on the electrocatalytic properties of Co 3 X 4 , and Co 3 Se 4 showed the strongest electrocatalytic activity for the oxidation of glucose. The sensor based on Co 3 Se 4 exhibited excellent performance for glucose analysis with a linear range from 2 μM to 0.71 mM, a high sensitivity of 1327.6 μA mM −1 cm −2 and a low detection limit of 0.3 μM, which demonstrates Co 3 Se 4 as a new nonenzymatic electrocatalyst for glucose sensing.
研究领域:
材料科学
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电化学
·
分析化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
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IF 8.758
Yanan Wang,Shuguang Zhang,Xiuxia Meng,Ting Wang,Yu Feng,Weimin Zhang,Yu-Shi He,Yucheng Huang,Naitao Yang,Zi-Feng Ma
Heterogeneous electrocatalytic reactions only occur at the interface between the electrocatalyst and reactant. Therefore, the active sites are only necessary to be distributed on the surface of the electrocatalyst. Based on this motivation, here, we demonstrate a systematic study on surface tuning for a carbon-based electrocatalyst from metal-free (with the heteroatoms N and S, NS/C) to metal-containing surfaces (with Co, N, and S, CoNS/C). The CoNS/C electrocatalyst was obtained by pyrolyzing the Co precoordinated and p-toluenesulfonate-doped polypyrrole (PPy). It was found that the coordination of Co on the PPy ring tuned the final carbon electrocatalyst into a catalyst with a CoNx moiety-rich surface. In addition, the as-synthesized CoNS/C was determined to have a very high loading of cobalt up to 2.02 wt %. The pyrolysis of the cobalt-containing precursor tends to proceed toward a characteristic of a higher sp2 carbon content, a higher surface area, and more nitrogen as well as active nitrogen sites than its metal-free counterpart. The most distinguished feature for such a catalyst is that the truly most active component is only distributed on the surface, in contrast with that of the conventional metal–N-based catalyst present throughout the bulky structure. Especially, the electrocatalytic activity toward oxygen evolution reaction (OER) has been investigated experimentally and theoretically. The results showed that the OER performance of the carbon-based electrocatalyst was remarkably boosted after the introduction of Co with an overpotential decrease from 678 to 345 mV at 10 mA cm–2. Furthermore, CoNS/C displayed an excellent durability upon a long-term measurement. The apparent activation energy measurements revealed that the metal-rich surface contributed to overcome the energy barrier for OER. In addition, density functional theory calculations have been conducted to explain the correlated OER mechanism. This study is expected to provide an effective strategy for the design and the synthesis of highly active metal–nitrogen-type electrocatalysts with a high metal loading for various electrocatalytic reactions.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Yi Han,Hongdong Li,Mingjuan Zhang,Yunlei Fu,Yanru Liu,Yu Yang,Jixiang Xu,Yanling Geng,Lei Wang
The development of relatively inexpensive and highly active electrocatalyst for water splitting is essential to the energy conversion and sustainable economic improvement. In this work, based on nanostructure engineering, the CoSe 2 -Ni 3 Se 2 nanoparticles coated Co(CO 3 ) 0.5 (OH)·0.11H 2 O nanoneedles supported on the surface of Ni foam (NF) composite (CoSe 2 -Ni 3 Se 2 /NF) had been synthesized by a facile hydrothermal selenization method. Benefiting from the adequate nanostructure and moderate degree of selenization treatment, the obtained sample CoSe 2 -Ni 3 Se 2 /NF-0.4 using 0.4 g Se powder as selenium source shows remarkable electrocatalytic performance and electrochemical stability for either hydrogen evolution reaction (HER) or oxygen evolution reaction (OER). CoSe 2 -Ni 3 Se 2 /NF-0.4 only required 98 mV (vs. RHE) to reach the 10 mA cm −2 for HER and 344 mV (vs. RHE) to reach 100 mA cm −2 for OER in 1.0 M KOH solution. This work provides a simple strategy to controllably synthesize transitional metal diselenium-based electrocatalyst with adjustable amount of active phase, which are very important for the future development of the bifunctional electrocatalyst.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
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2020
·Vol. 7
·期 10
·2006-2016
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IF 5.958
Yu Qiu,Sen Zhao,Mingxin Qin,Jinxiang Diao,Shuangquan Liu,Lanxin Dai,Wenhua Zhang,Xiaohui Guo
The conventional Haber–Bosch process dominates the production of industrial NH3, and unfortunately leads to a large amount of energy consumption and carbon dioxide emissions. Meanwhile, from the environmentally friendly and energy-saving point of view, electrocatalytic N2 fixation is gradually becoming a more promising and desirable alternative technique. Herein, multi-yolk–shell bismuth@porous carbon (MB@PC) composites were successfully synthesized via a facile simple hydrothermal reaction followed by a subsequent pyrolyzation. The as-prepared MB@PC composite can act as an efficient N2 reduction reaction (NRR) electrocatalyst under ambient conditions. Test results demonstrated that the MB@PC composite catalysts can deliver a high NH3 yield of 28.63 μg h−1 mg−1cat., a Faraday efficiency of 10.58% at −0.5 V versus a reversible hydrogen electrode, long-term electrochemical durability in N2-saturated 0.1 M HCl solution, and an excellent selectivity for NH3 formation, and are better than most reported bismuth-based electrocatalysts. The excellent NRR performance is mainly ascribed to the synergetic effect of good conductivity, the highly porous feature derived from the carbon framework and intrinsic electrocatalytic NRR activity of bismuth nanoparticles. Generally, the present research findings would provide an alternative avenue to produce other efficient non-precious metal electrocatalysts for clean energy applications.
研究领域:
材料科学
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能源化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2019
·
IF 7.723
Jinxi Feng,Jingxiang Sun,Xiaosheng Liu,Jinzhu Zhu,Shuanghong Tian,Rong Wu,Ya Xiong
Piezocatalysis is an emerging green advanced-oxidation technology for the degradation of toxic pollutants; however, piezomaterials are not generally excellent electrocatalysts. Herein, two complex piezocatalysts (SnO 2 / t -BaTiO 3 and SnO 2 -Sb/ t -BaTiO 3 ) consisting of an electrocatalyst and piezomaterial, respectively, are designed to investigate the coupled effect of piezocatalytic and electrocatalytic processes on the degradation of pollutants. SnO 2 , especially SnO 2 -Sb, can considerably enhance the piezocatalytic degradation of the antibiotic metronidazole (MNZ). The piezocatalytic rate constants of SnO 2 / t -BaTiO 3 and SnO 2 -Sb/ t -BaTiO 3 are 2.3 and 3.0 times that of t -BaTiO 3 , respectively. In the degradation process, SnO 2 and SnO 2 -Sb are confirmed to act as dimensionally stable anode-like (DSA-like) catalysts because they can increase the response of the piezoelectrochemical anodic current and the generation of OH radicals as well as reduce the formation of 1 O 2 . Significantly, the piezoelectric field can drive not only the free charges of t -BaTiO 3 and its remnant piezoelectric field but also those of the loaded electrocatalyst SnO 2 to participate in the degradation of MNZ. These results indicate that the coupling of an excellent electrocatalyst and piezomaterial is an effective method to promote piezocatalytic efficiency.
研究领域:
环境科学
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材料科学
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催化化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2016
·
IF 3.205
Lin Chen,Hao Hua,Qi Yang,Muhammad Sufyan Javed,Chenguo Hu,Cuiling Zhang
TiO 2 microflowers assembled by nanosheets are prepared by a one-step solvothermal process. The anatase-TiO 2 (B) dual-phase coexistence or anatase single phase is obtained under different annealing temperatures. Pt nanoparticles supported on the anatase-TiO 2 (B) microflowers are first applied to alcohol electrooxidation . The electrocatalytic performances of Pt/anatase-TiO 2 (B), Pt/anatase and Pt/carbon-black (Pt/C) on graphite substrates are systematically investigated. The Pt/anatase-TiO 2 (B) catalyst exhibits superior electrocatalytic activity and stability compared with that of Pt/anatase and Pt/C catalysts for methanol and ethanol in acidic and alkaline media , which is attributed to the large specific surface area, the porous channels to reduce the liquid sealing effect, the enhanced electronic conductivity by dual-phase coexistence and quick electron transfer from anatase phase to TiO 2 (B).
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Ya Zhang,Lang Hu,Yongcai Zhang,Xiaozhi Wang,Honggui Wang
Snowflake-like Cu 2 S/MoS 2 heterostructures with varied compositions were constructed via a two-step hydrothermal method. The 45-Cu 2 S/MoS 2 with 45 wt% Cu 2 S was found as the optimum catalyst, which displayed photothermal enhanced hydrogen evolution reaction (HER) performance under near infrared (NIR) irradiation. After electrochemical deposition of a tiny amount of Pt (45-Cu 2 S/MoS 2 /Pt-100s), Schottky barrier was formed between Pt nanoparticles and MoS 2 nanosheets . Using 45-Cu 2 S/MoS 2 /Pt-100s as an electrocatalyst, low overpotential of 78 mV (@10 mV cm −2 ) and Tafel slope of 48 mV dec −1 were achieved with the assistance of NIR irradiation. The photoelectrochemical (PEC) hydrogen production performance of 45-Cu 2 S/MoS 2 /Pt-100s was also investigated. The optimal conversion efficiency of 45-Cu 2 S/MoS 2 /Pt-100s could reach 0.78% at 0.57 V (vs. reversible hydrogen electrode (RHE)). The control of the internal geometric and electronic structure of the catalysts and the aid of photothermal effect in this work provide new ideas for designing high-efficiency hydrogen evolution catalysts.
研究领域:
材料科学
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能源化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xuran Mao,Yanbing Huang,Yue Xiao,Xun Liu,Yan Pei,Qianwen Chen,Xiruo Wang,Wen Guo,Hongbing Yang,Fuxi Bao
Developing highly efficient and robust electrocatalysts to enhance the kinetics of electrochemical nitrate reduction reaction (NO 3 RR) to ammonia is crucial for realizing the conversion and storage of green electrochemical ammonia energy. Herein, we constructed a molybdenum-doped metallic copper electrocatalyst (Cu-Mo 0.2 /NF) and systematically investigated the pivotal role of molybdenum dynamic recombination in enhancing the kinetics of the NO 3 RR. In situ Raman spectroscopy, XPS and ICP-OES reveals that Mo dissolves during the NO 3 RR process and recombines into Mo 2 O 7 2- species, which are adsorbed onto the surface of the electrocatalyst. The experimental results combined with DFT calculations indicates that this dynamic dissolution, reorganization, and adsorption process of Mo significantly activates *NO 3 , thereby greatly enhancing the kinetics of *NO 3 reduction to *NO 2 . Furthermore, Differential electrochemical mass spectrometry (DEMS) and in situ attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR) elucidate the NO 3 RR pathway: *NO 3 → *NO 2 → *NO → *NOH → *N → *NH → *NH 2 → *NH 3 . This reaction mechanism, which circumvents high-energy-barrier step (NO → N 2 O), endows the electrocatalyst with superior kinetics and high selectivity. Benefiting from the dynamic dissolution and redeposition of Mo and the advantages of the reaction pathway, the electrocatalyst achieves a record ammonia yield ( 1.55 mmol h −1 cm −2 ) with near-unity Faradaic efficiency ( 98.99 % ), and 30 h stability.
研究领域:
电催化
·
能源化学
·
材料科学
·
环境修复
·
可持续能源
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Xu Yang,Rui Qiu,Ming-Jian Lan,Gang Chen,Wei Xu,Yu Shen
Designing the efficient, low-cost and stable electrocatalyst is of great significance for storage and conversion of the renewable energy to hydrogen. Herein, the binder-free Ni–Fe–S electrocatalysts were directly electrodeposited on Ni foam, which exhibited the excellent hydrogen evolution reaction performance with the overpotential of 51.4 mV at the current density of 10 mA cm −2 . Based on the analysis and results of as-synthesized Ni, Ni–Fe and Ni–S, the boosted electrocatalytic activity can be attributed to the composite effect between Ni and the introduced Fe and S. Additionally, the Ni–Fe–S electrocatalysts also displayed the low cell voltage (1.59 V at 10 mA cm −2 ), remarkable durability and high Faraday efficiency in overall water electrocatalysis . Moreover, the water electrolysis device with Ni–Fe–S bi-electrodes can be driven by a small wind power generation and producing 4 mL H 2 in 39 min, indicating the prepared Ni–Fe–S electrocatalyst has the great potentials in producing hydrogen via renewable energy.
研究领域:
材料科学
·
能源转换与存储
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Yiming Li,Zheng Yan,Qiaodi Wang,Huating Ye,Mengli Li,Lianwen Zhu,Xuebo Cao
Metal-free heteroatom-doped porous carbons such as N, P co-doped nanoporous carbon materials with designed properties are attracting increased attention for metal-air battery applications. Herein, we report a general approach to synthesizing highly branched N, P co-doped carbon nanotube cluster (NPCTC) derived from metal-organic frameworks as a bifunctional electrocatalyst . NPCTC were obtained by treating ZIF-8 with butyl methylphosphinate, followed by two-step pyrolysis . Benefiting from the cross-linking polymerization and self-aggregation between ZIF-8 and the monomer , the resulting NPCTC exhibited higher mechanical stability and strength. Although the wall thickness was <5 nm, no obvious shrinkage and collapse were observed after graphitization, thereby maximizing the exposure of the active sites. Studies of oxygen electrocatalysis demonstrate that the NPCTC can deliver outstanding bifunctional performance with a more positive half-wave potential, higher limiting current density for oxygen reduction reaction (ORR) than Pt/C, and lower onset potential for oxygen evolution reaction (OER) than IrO 2 . Homemade Zn-air battery exhibited stable charge-discharge durability over 180 cycles, with an overpotential increase of only 0.15 V. The improved electrochemical performance was mainly attributed to the synergistic effect of N, P co-doping and the distinct geometry of NPCTC, i.e., three-dimensionally interconnected hollow ultrathin nanotube branches facilitating electron and mass transfer.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）