APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
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IF 24.319
Ning An,Lei Zhou,Wenli Li,Xiaoli Yuan,Li Zhao,Jingwei Huang,Yang Zhang,Houde She,Lei Wang,Qizhao Wang
Modifying semiconductor photoanode with efficient and cheap iron-based oxygen evolution cocatalyst along with functional interlayer is an efficient method to enhance the water splitting efficiency of photoelectrochemical (PEC). Poly-aminoanthraquinone (PDAAQ) due to its outstanding reversible redox activity plays a significant role as proton receptor. Herein, an easy-handle solvothermal method is adopted to prepare γ-Fe 2 O 3 -PDAAQ@BiVO 4 . With the concerted efforts of the ternary structure, the photocurrent of γ-Fe 2 O 3 -PDAAQ@BiVO 4 photoanode reach to 5.35 mAcm 2 at 1.23 V RHE (3.3 times of pure BiVO 4 ). The improvement is ascribable to the abundant catalytic active sites and large catalytic area of γ-Fe 2 O 3 nanoparticles . Additionally, theoretical calculations show that PDAAQ can form type II heterojunction with BiVO 4 to inhibit carrier recombination. At the same time, the role of PDAAQ in promoting water oxidation kinetics by accelerating proton coupled electron transfer process has also been confirmed in isotope effect experiment.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Chemistry-An Asian Journal
·
2017
·Vol. 12
·期 17
·2304-2310
·
IF 4.083
Wei Su,Kui Zhou,Fanglin Cai,Cheng Chen,Bibimaryam Mousavi,Somboon Chaemchuen,Francis Verpoort
Graphical Coordination configuration matters : A Ru dimer, [Ru(NC NHC O)(pic) 2 ] 2 2+ ( 2 ), which transforms to two single-site Ru-OH 2 species to initiate water oxidation, was prepared and fully characterized. Complex 2 could catalyze water oxidation electrochemically, chemically and photochemically, exhibiting an excellent reactivity and stability. A dinuclear ruthenium complex [Ru II (NC NHC O)(pic) 2 ] 2 2+ ( 2 ) was firstly prepared and characterized spectroscopically and electrochemically. Instead of the conventional ligand exchange, complex 2 dissociates in situ to afford two single-site Ru aqua complexes, [Ru II (OH 2 )(NC NHC O)(pic) 2 ] + , which mediates water oxidation through proton-coupled electron transfer events. In electrokinetic studies, complex 2 demonstrated a TOF of 150.3 s −1 comparable to those state-of-the-art catalysts at neutral conditions. TONs of 2173 and 217 were attained in chemical and photochemical water oxidation when 2 was used as a catalyst, exhibiting good stability. Notably, a TOF of 1.3 s −1 was achieved at CAN-driven water oxidation, which outperformed most of the reported single-site Ru complexes, indicating that complex 2 is one of most active water oxidation catalysts (WOCs) to date. The unique coordination configuration and outstanding catalytic performance of complex 2 might shed light on the design of novel molecular WOCs.
研究领域:
无机化学
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催化化学
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能源化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xin Guo,Longyu Qiu,Menggang Li,Fenyang Tian,Xue Ren,Sheng Jie,Shuo Geng,Guanghui Han,Yarong Huang,Ying Song,Weiwei Yang,Yongsheng Yu
Nickel sulfide (Ni 3 S 2 ) is a highly promising electrocatalyst for urea oxidation reaction (UOR), and NiOOH formed by the surface phase transition of Ni 3 S 2 during UOR is the ideal catalytic active species. However, the strong covalent bonds of Ni 3 S 2 hinders the generation of NiOOH, limiting the further improvement of UOR activity. Herein, the Ni 3 S 2 @Ni 3 P core–shell nanorods have been constructed by an in-situ surface phosphating method to boost UOR performance, realizing high catalytic activity (100/1000 mA cm −2 at 1.36/1.49 V vs . RHE, respectively) and a rapid kinetics (19.13 mV dec -1 ). The Ni 3 P on the surface of Ni 3 S 2 can rapidly form highly active γ-NiOOH with low energy consumption, and the formed Ni 3 S 2 @γ-NiOOH accelerates proton-coupled electron transfer (PCET) kinetics through reducing the energy barrier of urea dehydrogenation process, thereby enhancing UOR intrinsic activity. In addition, we also demonstrate a Ni 3 S 2 @Ni 3 P//Ni 3 S 2 @Ni 3 P urea electrolysis device with low voltages of 1.54 and 1.69 V at current densities of 100 and 500 mA cm −2 , respectively. This work proposes an efficient strategy to accelerate the generation of NiOOH on the surface of Ni 3 S 2 during UOR electrocatalysis, revealing the enhanced UOR mechanism of Ni 3 S 2 @Ni 3 P, which can promote the development of urea-assisted hydrogen production .
研究领域:
电化学
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催化材料
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能源转换与储存
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Hui Feng,Yue Han,Yutong Wang,Dong-Feng Chai,Jianxin Ran,Wenzhi Zhang,Zhuanfang Zhang,Guohua Dong,Meili Qi,Dongxuan Guo
Traditional phase engineering enhances conductivity or activity by fully converting electrocatalytic materials into either a crystalline or an amorphous state, but this approach often faces limitations. Thus, a practical solution entails balancing the dynamic attributes of both phases to maximize an electrocatalyst’s functionality is urgently needed. Herein, in this work, Co/Co 2 C crystals have been assembled on the amorphous N, S co-doped porous carbon (NSPC) through hydrothermal and calcination processes. The stable biphase structure and amorphous/crystalline (A/C) interface enhance conductivity and intrinsic activity. Moreover, the adsorption ability of water molecules and intermediates is improved significantly attributed to the rich oxygen-containing groups, unsaturated bonds, and defect sites of NSPC, which accelerates proton-coupled electron transfer (PCET) and overall water splitting. Consequently, A/C-Co/Co 2 C/NSPC (Co/Co 2 C/NSPC with amorphous/crystalline interface) exhibits outstanding behavior for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), requiring the overpotential of 240.0 mV and 70.0 mV to achieve 10 mA cm −2 . Moreover, an electrolyzer assembled by A/C-Co/Co 2 C/NSPC-3 (anode) and A/C-Co/Co 2 C/NSPC-2 (cathode) demonstrates a low drive voltage of 1.54 V during overall water splitting process. Overall, this work has pioneered the coexistence of crystalline/amorphous phases in electrocatalysts and provided new insights into phase engineering.
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
Small
·
2024
·Vol. 20
·期 38
·2403310
·
IF 13
Jing Qi,Qizhen Chen,Mingxing Chen,Wei Zhang,Xinxin Shen,Jing Li,Enbo Shangguan,Rui Cao
Understanding the structure-activity correlation is an important prerequisite for the rational design of high-efficiency electrocatalysts at the atomic level. However, the effect of coordination environment on electrocatalytic oxygen evolution reaction (OER) remains enigmatic. In this work, the regulation of proton transfer involved in water oxidation by coordination engineering based on Co 3 (PO 4 ) 2 and CoHPO 4 is reported. The HPO 4 2− anion has intermediate p K a value between Co(II)-H 2 O and Co(III)-H 2 O to be served as an appealing proton-coupled electron transfer (PCET) induction group. From theoretical calculations, the pH-dependent OER properties, deuterium kinetic isotope effects, operando electrochemical impedance spectroscopy (EIS) and Raman studies, the CoHPO 4 catalyst beneficially reduces the energy barrier of proton hopping and modulates the formation energy of high-valent Co species, thereby enhancing OER activity. This work demonstrates a promising strategy that involves tuning the local coordination environment to optimize PCET steps and electrocatalytic activities for electrochemical applications. In addition, the designed system offers a motif to understand the structure-efficiency relationship from those amino-acid residue with proton buffer ability in natural photosynthesis.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 63
·39985-39993
·
IF 3.361
Yirong Xia,Xintong Wang,Hechen Sun,Ximing Huang
Tea wine is a Chinese traditional alcoholic drink made by cereal and tea leaves. It is rich in tea polyphenols, caffeine, amino acids, and protons and possesses various healthcare functions. In this work, electrochemical methods, as well as density functional theory (DFT) calculations, were adopted to reveal the proton-coupled electron-transfer process of catechin in tea wine. The electrochemical results showed that the catechin preferred hydrogen-bonding with ethanol and formed molecular clusters. Thus, the direct electron-transfer process of catechin changed to proton-coupled electron transfer. This procedure reduced the energy barrier of the redox reaction and enhanced the anti-oxidative capacity. Subsequently, DFT calculations were employed to explore the bond length, bond energy, and HOMO–LUMO energy gap of catechin, which confirmed the above-mentioned mechanism. Our work offers some positive value for the scientific promotion of traditional food and a greater understanding of the health mechanisms in terms of chemistry.
研究领域:
食品科学
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电化学
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计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Wenchuan Jiang,Wenrui Liu,Yunpeng Wang,Zhiyu Zhao,Qing Li,Yifan Wu,Tao Liu,Heping Xie
Electrochemical CO2 capture driven by a proton-coupled electron transfer (PCET) reaction, exploiting the CO2 hydration/dehydration equilibrium through pH swing, has the potential for low-energy capture as it eliminates the sensible heat from the temperature-swing process. However, carbonate salts used in the pH swing method suffered from poor reaction kinetics and crystal accumulation, which could potentially clog electrodes and become electrically disconnected. While amines are widely applied in various methods as efficient capturing agents, their capture energy consumption is generally higher than 100 kJ/mol CO2. Here, we propose a scheme of electrochemical CO2 capture driven by a PCET reaction using amines instead of carbonates as CO2 capture agents. In this scheme, H+ generated by the PCET reaction will promote CO2 desorption from the amine–CO2 compound, and the CO2 absorption of amines can be achieved through the consumption of H+ by the PCET reaction. Furthermore, we establish a thermodynamic model of the energetic cost of the method by introducing a multibuffer system of amines, showing that the introduction of amines will moderate the pH swing during the four-stage cycle, resulting in a 45.2% reduction in theoretical CO2 capture energy consumption compared to carbonate. Besides, we validated the model and obtained an experimental energy cost of 21.0 kJe/mol with 0.15 bar CO2 (g) captured using a hydrogen cycle. We expect that this strategy of introducing a multibuffer system to reduce CO2 capture energy consumption could provide a reference for low-energy consumption electrochemical CO2 capture in the future.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Lingzhe Meng,Shuwen Niu,Zhengyu Wei,Xue Qin,Faheem Naseem,Wei Wei
Iron phthalocyanine (FePc) with tetracoordinated Fe-N 4 site shows promising activity for catalyzing the oxygen reduction reaction (ORR) in alkaline media. However, the consecutive proton-coupled electron transfer (PCET) steps with water as the proton donor and low electronic conductivity of FePc raise the kinetic barriers for device application. Herein, a significant effect of polyoxometalates (POMs) on the ORR kinetics of Fe-N 4 sites via surface coordination of FePc is revealed. POM clusters modulate the interactive steric/electronic environment of Fe-N 4 , leading to a low barrier for H 2 O cleavage to produce protons along with a high electron transfer rate, thereby accelerating the PCET steps of FePc. With precisely controlled electron charge of POM clusters, the influence and mechanism of heteropoly blue in promoting PCET steps of FePc relative to heteropoly acid are elucidated, and noticeably enhanced ORR activity and reaction current are achieved. These findings highlight the potential of POMs as ligands to optimize dynamics of Fe-N 4 atomic sites toward efficient alkaline ORR.
研究领域:
化学
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2015
·
IF 4.772
Yaofang Xuan,Xiao Huang,Bin Su
An investigation of oxygen reduction reaction (ORR) catalyzed by microperoxidase-11 (MP-11) at the polarized water/1,2-dichloroethane (DCE) interface is reported. MP-11 contains a heme group covalently bonded to an undecapeptide chain via two thioether bonds of cysteine residues, as in cytochrome c oxidases (CcOs), and has been widely studied as a biomimetic model of CcOs. Herein we demonstrated that MP-11 can adsorb at the water/DCE interface and catalyze the O2 reduction by lipophilic electron donors, namely tetrathiafulvalene (TTF) and 1,1′-dimethylferrocene (DFc). The overall catalytic ORR corresponds to a proton coupled electron transfer (PCET) reaction and is kinetically controlled by the heterogeneous conversion of MP-11 from ferric (FeIII-MP-11) to ferrous state (FeII-MP-11). Given that a significant amount of H2O2 was produced for both electron donors, it indicates that MP-11 has a remarkable impact on the ORR pathway and that MP-11, similar to other mononuclear macrocyclic compounds, cannot selectively catalyze the 4e–/4H+ reduction of O2 to H2O. The results also suggest that one should carefully considers the role of Cu site in CcOs and the reaction environment to understand respiratory ORR and to develop more selective catalysts for practical applications (e.g., fuel cells).
研究领域:
生物化学
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电化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Feng Zhao,Yimin Deng,Miyi Li,Can Lv,Tejraj M. Aminabhavi,Ozge Yuksel Orhan,Helei Liu
The CO 2 desorption in amine-based carbon capture processing is accompanied by significant energy consumption, accounting nearly 70% of energy requirements of the entire process. Electrochemical CO 2 capture and release are promising technologies to reduce the energy consumption. The characteristics and CO 2 desorption performance of QH 2 (Tiron) in tertiary amine systems are investigated in this research. The reducing ability of Q (Oxidized QH 2 ) was improved by modifying the electrode to achieve low-energy electrochemical desorption. The CO 2 electrochemical desorption achieved low-energy CO 2 desorption of 0.7 GJ ton −1 CO 2 against over 2.4 GJ ton −1 in a conventional and mature MEA-based system.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
iScience
·
2022
·
IF 6.107
Cong Niu,Jianjing Yang,Kelu Yan,Jiafang Xie,Wei Jiang,Bingwen Li,Jiangwei Wen
A straightforward and practical strategy for pyridylation of inert N-heterocycles, enabled by ammonium cation and electrochemical, has been described. This protocol gives access to various N-fused heterocycles and bidentate nitrogen ligand compounds, through dual-proton-coupled electron transfer (PCET) and radical cross-coupling in the absence of exogenous metal and redox reagent. It features broad substrate scope, wide functional group tolerance, and easy gram-scale synthesis. Various experiments and density functional theory (DFT) calculation results show the mechanism of dual PCET followed by radical cross-coupling is the preferred pathway. Moreover, ammonium salt plays the dual role of protonation reagent and electrolyte in this conversion, and the resulting product 9-(pyridin-4-yl)acridine compound can be used for fluorescence recognition of Fe 2+ and Pd 2+ with high sensitivity.
研究领域:
有机化学
·
材料科学
·
分析化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yao Shen,Ke Wang,Lu Li,Jingkai Zhao,Jiexu Ye,Ping Chen,Xiang Gao,Shihan Zhang
Catalyst-aided CO 2 desorption offers a promising reduction in the energy penalty of amine scrubbing, but faces the challenges of slow mass transfer, sluggish desorption kinetics, and susceptibility to deactivation. In this work, a hollow composite catalyst C@ZrO 2 was developed to simultaneously realize rapid electron, proton and mass transfer for CO 2 desorption via facilitating proton-coupled electron transfer (PCET) effect. The CO 2 desorption rate of benchmark MEA solution increased by 126% and relative heat duty decreased by 69.9% in presence of C@ZrO 2 , and its catalytic performance didn’t noticeably decline after 10 cycles. Additionally, the desorption rate of biphasic solvents with a high viscosity increased by 112% and relative heat duty decreased by 57.3% with C@ZrO 2 . Based on theoretical calculation, the facilitated PCET efficiency of carbon layer increased the binding energy of carbamate to enhance its mass transfer rate from the liquid phase to the C@ZrO 2 surface, and stretched the C-N bond to reduce the proton transfer energy barrier by 66.8%. This work provided a novel insight to design catalysts for energy-efficient and stable CO 2 capture.
研究领域:
化学工程
·
催化材料
·
环境科学
✓ 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）