ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Karuppasamy Kohila Rani,Qiong Yang,Yuan-Hui Xiao,Rajkumar Devasenathipathy,Zhihao Lu,Xinya Chen,Lu Jiang,Zemin Li,Qinghua Liu,Haonan Chen,Liuyingzi Yu,Zhuoyao Li,Soukaina Khayour,Junjie Wang,Kaili Wang,Gongqiang Li,De-Yin Wu,Gang Lu
Plasmon-mediated electrochemistry is an emerging area of interest in which the electrochemical reactions are enhanced by employing metal nanostructures possessing localized surface plasmon resonance (LSPR). However, the reaction efficacy is still far below its theoretical limit due to the ultrafast relaxation of LSPR-generated hot carriers. Herein, we introduce p-hydroxythiophenol (PHTP) as a molecular cocatalyst to significantly improve the reaction efficacy in plasmon-mediated electrochemical oxidation of p-aminothiophenol (PATP) on gold nanoparticles. Using electrochemical techniques, in situ Raman spectroscopy, and theoretical calculations, we elucidate that the presence of PHTP improves the hot hole-mediated electrochemical oxidation of PATP by 2-fold through the trapping of plasmon-mediated hot electrons. In addition, the selectivity of PATP oxidation could also be modulated by the introduction of PHTP cocatalyst. This tactic of employing molecular cocatalyst can be drawn out to endorse various plasmonic electrochemical reactions because of its simple protocol, high efficiency, and high selectivity.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Shuangchi Li,Ning Wang,Shuiqing Chen,Yuqing Sun,Puwang Li,Jinfang Tan,Xiaoqian Jiang
Phosphate fertilizers have been excessively applied in agricultural production, bringing the risk of phosphorus (P) loss to nearby river systems and low utilization efficiency. In this study, eggshell-modified biochars prepared by pyrolysis of eggshell and corn straw or pomelo peel were applied to soil for enhancing P immobilization and utilization. The structure and properties of modified biochars before and after P adsorption were analyzed using the Brunauer-Emmett-Teller (BET) nitrogen adsorption method, Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and scanning electron microscope (SEM). The eggshell-modified biochar performed an excellent adsorption performance for P (up to 200 mg/g), which was well described by the Langmuir model (R 2 > 0.969), showing monolayer chemical adsorption with homogenous surface. The Ca(OH) 2 appeared on the surface of eggshell modified biochars and changed to Ca 5 (PO 4 ) 3 (OH) and CaHPO 4 (H 2 O) 2 after P adsorption. The release of immobilized P by modified biochar increased with decreased pH. In addition, pot experiments of soybean indicated that the combined application of modified biochar and P fertilizer significantly increased the content of microbial biomass P in soil, raising from 4.18 mg/kg (control group) to 51.6–61.8 mg/kg (treatment group), and plants height increased by 13.8–26.7%. Column leaching experiments showed that P concentration in the leachate decreased by 97.9% with the modified biochar application. This research provides a new perspective that the eggshell-modified biochar could serve as a potential soil amendment for enhancing P immobilization and utilization.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2023
·Vol. 25
·期 7
·1-16
·
IF 2.5
Shan Chuanfu,Liu Ziyi,Li Fuchao,Jia Wenhan,Cai Gaotuo,Li Ming,Tang Tao,Li Shuai,Wen Jianfeng,Hu Guanghui,Jiang Li,Li Xinyu
TiO 2 -based materials are important photocatalysts but the rapid recombination of photoexcited electron–hole pairs, and the wide band gap both limit their photocatalytic activities. In this work, p-type phosphorus-doped graphene quantum dots (P-GQDs, 5~20 nm) were combined with n-type TiO 2 nanoparticles (20~50 nm) and n-type silver iodide (AgI, 100~200 nm) by a facile sonication and precipitation process to yield a novel ternary photocatalyst TiO 2 /P-GQDs/AgI with n-p-n heterojunctions. The morphologies, structures, optical properties, and chemical environments of photocatalysts were all studied. The resulting ternary photocatalyst exhibited enhanced visible photocatalytic activity toward the degradation of methyl orange (MO), estimated to 70.4-fold that of pure TiO 2 . By contrast, the photocatalytic activities of TiO 2 /GQDs with an n-n heterojunction, TiO 2 /P-GQDs with a p-n heterojunction, and TiO 2 /GQDs/AgI (30%) with an n-n-n heterojunction showed 4.4-fold, 5.3-fold, and 14.2-fold higher than those of TiO 2. The electrochemical and optical measurements revealed that the enhanced photocatalytic activity was linked to promoted charge carrier separation by n-p-n heterojunctions coupled with the increased absorption in the visible region. Overall, the new band structure connected in series p-n heterojunctions looks promising as a highly efficient photodegradation system for future use in decontamination of polluted water. Graphical abstract
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Bo Pei,Yinmei Li,Shenhui Ma,Yuyu Bu
The photoelectrochemical (PEC) water splitting performance of Si-based PEC devices is usually restricted by low stability and weak photogenerated carrier transport ability. Herein, a micropyramid array structure (p-SiMPs)/p-Cu2O/PhC2Cu/Pt photocathode device with a p-p-n heterojunction structure is developed. In this tandem PEC device, a p-p heterojunction of p-SiMPs/p-Cu2O is achieved, endowing a higher interface electric field and stronger energy of photoinduced electrons for PEC water reduction. In addition, a stable n-type PhC2Cu protective layer is prepared on the surface of the PEC device by the photoassisted polymerization method, which can improve the stability of PEC water reduction largely. After Pt cocatalytic layer deposition, the p-SiMPs/p-Cu2O/PhC2Cu/Pt tandem photocathode can achieve a saturation photocurrent density of −30 mA/cm2 at −0.9 V (vs RHE) and a photocurrent threshold voltage of −0.1 V for water reduction. This work provides a silicon-based p-p-n heterojunction tandem structure for the PEC water splitting; meanwhile, it indicates that PhC2Cu is a potential material to improve the stability of silicon-based PEC devices.
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Nature Catalysis
·
2023
·Vol. 6
·期 2
·174-184
·
IF 37.8
Hua Wuxing,Shang Tongxin,Li Huan,Sun Yafei,Guo Yong,Xia Jingyi,Geng Chuannan,Hu Zhonghao,Peng Linkai,Han Zhiyuan,Zhang Chen,Lv Wei,Wan Ying
Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p -block metal sulfides and the apparent activation energies ( E a ) for the sulfur reduction reaction (SRR), in particular, Li 2 S n to Li 2 S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest E a and a high SRR rate in the cathode. Li–S batteries with the Bi 2 S 3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm −2 was obtained under a high sulfur loading of 17.6 mg cm −2 but a low electrolyte/sulfur ratio of 7.5 μl mg −1 .
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Biology-Basel
·
2025
·Vol. 14
·期 10
·1358
·
IF 3.5
Bo Fan,Shunuan Fu,Yijun Zhu,Wei Tang,Yucai He
Simple SummaryThis study enhanced the relative activity of glycosyltransferase UGTBL1 through engineering mutations near its loop regions. The engineered enzyme efficiently catalyzed the glycosylation of the lignin-derived compoundp-hydroxybenzaldehyde (C7H6O2), enabling the environmentally benign synthesis of a Helicid analogue (p-hydroxybenzaldehydeβ-glucoside (C13H16O7)). Accordingly, this work provided novel insights for lignin valorization. Under optimized reaction conditions (35 °C, pH 7.5, 200 mM glucose (C6H12O6)), an exceptional yield of 97.8% forp-hydroxybenzaldehydeβ-glucoside was attained within 10 h using 2 mMp-hydroxybenzaldehyde substrate. Biotransformation of 3 mMp-hydroxybenzaldehyde (366.4 mg/L) afforded up to 2.7 mM of targetβ-glucoside product (767.5 mg/L). This research establishes a simpler, more economical, and sustainable enzymatic approach for the efficient synthesis ofp-hydroxybenzaldehydeβ-glucoside, offering significant potential benefits for pharmaceutical, cosmetic, or agricultural applications.Lignin, as one of the three primary components of renewable lignocellulosic biomass, can be converted into aromatic platform chemicals and holds significant potential for high-value applications.p-Hydroxybenzaldehyde is a compound derived from lignin. In this study, the mutant Δ60 of the glycosyltransferase UGTBL1 derived fromBacillus licheniformiswas adopted to catalyze the glycosylation reaction ofp-hydroxybenzaldehyde, producing a bioactive compound Helicid analogue (p-hydroxybenzaldehydeβ-glucoside). Truncation mutations targeting loop regions may reduce local flexibility, thereby facilitating enhanced access ofp-hydroxybenzaldehyde to the active site pocket and promoting relative activity. Under optimal conditions (35 °C, pH 7.5, and glucose 200 mM), a high yield of 97.8% forp-hydroxybenzaldehydeβ-glucoside was achieved from 2 mMp-hydroxybenzaldehyde within 10 h. The conversion of 3 mMp-hydroxybenzaldehyde (366.4 mg/L) yielded up to 2.7 mM (767.5 mg/L) ofp-hydroxybenzaldehydeβ-glucoside within 48 h. According to the molecular docking results, the CDOCKER energy value of mutant Δ60 was lower than that of the wild-type, at −16.0 kcal/mol. To our knowledge, this is the first example of an efficient and environmentally sustainable approach for the synthesis ofp-hydroxybenzaldehydeβ-glucoside, providing a new insight for the valorization of lignin into valuable biobased chemicals.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 38
·21766-21773
·
IF 10.733
Shixue Zhang,Huan Liu,Bin Cao,Qizhen Zhu,Peng Zhang,Xin Zhang,Renjie Chen,Feng Wu,Bin Xu
Two-dimensional transition metal carbides (MXenes) have a unique structure, excellent electronic conductivity and a low Li+ diffusion barrier, and show potential for application in energy storage. Especially, MXenes can act as a conductive matrix to achieve excellent lithium storage performance. Herein, a Ti3C2Tx MXene/carbon nanotubes@red phosphorus (Ti3C2Tx/CNTs@P) nanohybrid with stable Ti–O–P bonds is fabricated. The CNTs are introduced into Ti3C2Tx to construct a conductive network, and then the Ti3C2Tx/CNTs are combined with P by a ball-milling method. In this process, the surface oxygen-containing functional groups of Ti3C2Tx interact with P, forming Ti–O–P bonds. Owing to the large capacity contribution of P, the conductive network and buffering role of Ti3C2Tx/CNTs, and the effect of the Ti–O–P bond, the Ti3C2Tx/CNTs@P nanohybrid exhibits a superior reversible capacity of 2598 mA h g−1 at 0.05C (1C = 2600 mA g−1, based on the active material P), excellent cycling stability (2078 mA h g−1 after 500 cycles) and superior rate capability (454 mA h g−1 at 30C). These results demonstrate that the Ti3C2Tx/CNTs@P nanohybrid offers fascinating potential for high-performance lithium-ion batteries.
研究领域:
材料科学
·
储能
·
纳米技术
·
电化学
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ACS Nano
·
2026
·
IF 16
Kuo Sun,Ningxin Xiao,Shaojian Jiang,Kai Deng,You Xu,Ziqiang Wang,Liang Wang,Hongjie Yu,Hongjing Wang
Electrocatalytic alkynol semihydrogenation (EASH) represents a promising alternative to conventional alkenol production. However, it is plagued by severe overhydrogenation and a competitive hydrogen evolution reaction (HER). In this work, we synthesize a Pd3BiCx intermetallic carbide metallene (Pd3BiCx ene) as a high-performance electrocatalyst for the selective semihydrogenation of 2-methyl-3-butyn-2-ol (MBY). At −0.3 V vs RHE, the catalyst system achieves 94.1% conversion, 95.3% selectivity, and 90.4% Faradaic efficiency while maintaining long-term stability over 70 h. Mechanistic studies demonstrate that carbon doping induces synergistic p-d-p orbital hybridization among Pd, Bi, and C. This electronic structure modulation optimizes the adsorption energy of MBY while facilitating the desorption of 2-methyl-3-buten-2-ol (MBE). Furthermore, carbon doping kinetically hinders overhydrogenation by eliminating subsurface hydrogen species and increasing the energy barrier for the overhydrogenation step. Concurrently, this p-d-p hybridization stabilizes surface adsorbed hydrogen (H*ads), thereby promoting the hydrogenation pathway and suppressing the HER. This work establishes an effective catalyst design strategy for fabricating p-d-p orbital-hybridized intermetallic catalysts, offering an innovative approach for high-efficiency EASH.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Pengna Wang,Ying Sun,Jie Li,Guanqun Zhu,Xueqin Zhang,Hong Yang,Baoping Lin
Novel monomer TPACz containing carbazole and triphenylamine active groups was synthesized. P(TPACz)/WO 3 coralloid porous electrochromic electrode material were prepared by electropolymerization . The P(TPACz)/WO 3 coralloid porous composite electrode material exhibited independent electrochromic properties in the positive potential range (0−1.7 V) (yellow at neutral state and blue at oxidation state) and negative potential range (−1.8−0 V) with the color of the film changing from yellow to dark blue. At the same time, the electrochemical properties of P(TPACz)/WO 3 composite material ware tested. It is noteworthy that the P(TPACz)/WO 3 coralloid porous electrochromic composite electrode materials exhibit both n-type and p-type doped electrochemical properties . Especially, P(TPACz)/WO 3 exhibit excellent capacitive properties in the n-doped state. According to its GCD curve of P(TPACz)/WO 3 nanocomposite electrode material, the area ratio capacitance is 1.94 mF cm −2 in the positive potential window of 0−0.8 V. And the area ratio capacitance is 33.3 mF cm −2 in the negative potential window of −1.8−0 V. Therefore, the design and effects of the nanocomposite material can broaden application range of electrochromic electrode materials and provide new strategies for energy saving material design.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 47
·22672-22685
·
IF 3.925
Jing Wang,Mei Zhang,Feng Li,Huan Wang,Yanguang Chen,Hua Song
To deeply understand the role of P in hydrodeoxygenation (HDO), SiO2-supported Ni and Ni–P catalysts with different P/Ni ratios (x) were prepared. The as-prepared samples were characterized by various characterization methods. The HDO activity and product distribution over the Ni/SiO2 and N–P/SiO2-x were compared and the effects of x on the structure, acidity, formation mechanism of active phases and HDO performance were studied taking m-cresol HDO as a model reaction. The results showed that the introduction of P promotes the formation of smaller active sites and contributes to the creation of weak and medium strength acid sites through the formation of P–OH groups and Niδ+ in Ni2P. HDO over the Ni/SiO2 catalyst occurs mainly via the hydrogenation (HYD) route with 3-methyl-cyclohexanol (3-MCHnol) as the main product. However, for Ni–P/SiO2-x catalysts, methyl-cyclohexane (MCH) selectivity increases first and then decreases with the increase of x, reaching a maximum of 95% at x = 1. The acidity generated by the introduction of P contributes to increased MCH selectivity, while the dehydration of 3-MCHnol to MCH occurs mainly on acid sites. However, the excessively high P content (x ≥ 2.0) leads to a significant increase of MB (toluene) selectivity, which is associated with the increase in Ni(I) sites. About 100% m-cresol conversion was achieved with Ni–P/SiO2-1.0 when the m-cresol (g)/catalyst (g) ratio was 3, with MCH (99.4%) as the major product, showing great promise for deep HDO catalysis.
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ENERGY & FUELS
·
2023
·
IF 5.3
Huihua Wang,Wenchang Li,Jinhong Wu,Deyong Wang,Dong Hou,Minqi Sheng,Ruiqi Guo
Water splitting through electrolysis has been recognized as a promising solution for the production of hydrogen and oxygen to advance many renewable energy conversion and storage systems, while the key is the innovative exploration of cost-efficient electrocatalysts. Herein, interface-modified Ni–Fe–P/Co–P/NF alloys were achieved through a facile electroless plating strategy, in which the constructed interfaces benefited not only from the strong electron interaction but also from the fast mass transfer, significantly boosting the oxygen evolution reaction and hydrogen evolution reaction catalytic performance. More interestingly, water-splitting cells assembled using Ni–Fe–P/Co–P/NF-5L alloys as the cathode and anode, respectively, only requires a cell voltage of ∼1.52 V at 10 mA cm–2, far lower than that of the integrated Pt–C/NF and RuO2/NF couple (1.61 V). Also, the Ni–Fe–P/Co–P/NF-5L||Ni–Fe–P/Co–P/NF-5L system shows an outstanding durability over a long-term operation of 48 h at 10 mA cm–2. The work demonstrates an innovative strategy to construct heterogeneous interfaces for high-performance electrocatalysts and is suggested to be readily extended to regulate heterogeneous interfaces among other binary and ternary electrocatalysts, such as transition metal phosphides/borides, for scaling up water-splitting technology.
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DYES AND PIGMENTS
·
2024
·
IF 4.1
Di Wu,Yi Wang,Wenjing Qi,Jianyang Xu,Kanglin Pei,Lingyan Ma,Lin Qi
Long-lasting chemiluminescence of lucigenin/p-aminophenol (4-AP) system is explored for the first time and possible chemiluminescence enhancement mechanism is also proposed in this work. 4-AP can enhance chemiluminescence of lucigenin nearly 150 times and is stable for nearly 5 min, which overcomes the need of flow syringe pump. While o-aminophenol (2-AP) slightly enhances chemiluminescence of lucigenin and m-aminophenol (3-AP) does not. Thus, it can be applied in discrimination of three aminophenol isomers. More importantly, cyclic voltammetry proves the lowest oxidation peak for 4-AP at 115 mV, which is speculated to be the main reason for 4-AP induced chemiluminescence enhancement. It has been applied in chemiluminescence enhancement detection of 4-AP and p-nitrophenol (4-NP) from 80 nM to 60 μM, from 0.5 μM to 60 μM with limit of detection (LOD) of 26 nM and 0.17 μM, respectively. It shows high selectivity and anti-interference in chemiluminescence enhancment detection of 4-AP and 4-NP towards other organic compounds and metal ions. It also exhibits high accuracy in chemiluminescence enhancment detection of 4-AP and 4-NP in lake water with recoveries from 98.7% to 101.5% for and recoveries from 98.7% to 102.2%, respectively. It expands the study of long-lasting lucigenin chemiluminescence system and chemiluminescence method utilized in discrimination of aminophenols isomers.
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