ADVANCED MATERIALS
·
2023
·Vol. 35
·期 14
·2211790
·
IF 29.4
Xiang Miao,Wenxing Chen,Shuning Lv,Anran Li,Yanhong Li,Qinghua Zhang,Yonghai Yue,Hewei Zhao,Limin Liu,Shaojun Guo,Lin Guo
Precisely tailoring the oxidation state of single-atomic metal in heterogeneous catalysis is an efficient way to stabilize the single-atomic site and promote their activity, but realizing this approach remains a grand challenge to date. Herein, a class of stable single-atomic catalysts with well-tuned oxidation state of Pt by forming Pt Fe atomic bonds is reported, which are supported by defective Fe 2 O 3 nanosheets on reduced graphene oxide (PFARFNs). These as-synthesized materials can greatly enhance the catalytic activity, stability, and selectivity for the diboration of alkynes. The PFARFNs exhibit high conversion of 99% at 100 °C with an outstanding turnover frequency (TOF) of 545 h −1 , and a relatively high conversion of 58% at room temperature (25 °C) with a TOF of 310 h −1 , which has been hardly achieved previously. Through both experimental and theoretical investigation, it is demonstrated that the fast electron transfer from Fe to Pt in Fe–Pt–O atomic sites in PFARFNs can not only stabilize the single-atomic Pt, but also significantly improve their catalytic activity.
研究领域:
催化化学
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材料科学
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2021
·Vol. 17
·期 47
·2103778
·
IF 13.281
Huajin He,Ying Liao,Wenhua Zuo,Guochang Li,Jiabao Gu,Yixiao Li,Zheng Hu,Yong Yang
Reducing SF 6 (as gas cathode) in Li batteries is a promising concept for the double benefit of mildly converting greenhouse SF 6 and providing a high theoretical energy density of 3922 Wh kg −1 . However, the reduction process is hampered by its sluggish kinetics. Here, cobalt phthalocyanine (CoPc) molecules immobilized on porous carbon matrix are, for the first time, introduced to the Li SF 6 chemistry to deliver an enhanced energy density. It is revealed that the high redox potential of Co(II)Pc/[Co(I)Pc] − (≈2.85 V) facilitates the formation of Co(I) N 4 sites to catalyze the SF 6 electrochemical reduction. By using highly porous holey nitrogen-doped carbon nanocages as carbon matrix, the Li SF 6 cells deliver a high discharge voltage of 2.82 V at 50 mA g C+CoPc −1 and an unprecedented areal capacity of 25 mAh cm −2 at 0.1 mA cm −2 , much superior to previous results. This work opens up new possibilities for high-efficiency conversion of SF 6 in lithium batteries.
研究领域:
材料科学
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电化学
·
环境科学
✓ 已验证
DOI
高影响因子
Advanced Science
·
2023
·Vol. 10
·期 22
·2301869
·
IF 15.1
Zhiyong Jiang,Xiaodi Zhu,Zhiyu Wang,Wei Liu,Wensheng Yan,Kevin Sivula,Jun Bao
The structural properties of octahedral sites (B Oh ) in spinel oxides (AB 2 O 4 ) play vital roles in the electrochemical performance of oxygen-related reactions. However, the precise manipulation of AB 2 O 4 remains challenging due to the complexity of their crystal structure. Here, a simple and versatile molten-salt-mediated strategy is reported to introduce Ni 2+ in B oh sites intentionally on the surface of zinc ferrite (ZnFe 2 O 4 , ZFO) to promote the active sites for photoelectrochemical (PEC) water splitting. The as-created photoanode (ZFO-MSNi) shows a remarkable cathodic shift of ≈ 450 mV (turn-on voltage of ≈ 0.6 V RHE ) as well as three times the 1-sun photocurrent density at 1.23 V RHE for PEC water oxidation in comparison with bare ZFO. A comprehensive structural characterization clearly reveals the local structure of the introduced Ni 2+ in ZFO-MSNi. Fewer surface trapping states are observed while the precisely introduced Ni 2+ and associated neighboring Fe (3- σ )+ (0< σ <1) sites unite in an edge-sharing octahedral configuration to function as Ni Fe dual active sites for PEC water oxidation. Moreover, open circuit potential measurements and rapid-scan voltammetry investigation give further insight into the enhanced PEC performance. Overall, this work displays a versatile strategy to regulate the surface active sites of photoelectrodes for increasing performance in PEC solar energy conversion systems.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 10
·e18153
·
IF 3.7
Jiahui He,Suiqin Li,Chun Li,Kai Li,Yinjie Xu,Mengxin Wang,Shuying Zhao,Jiefeng Zhang,Xing Zhong,Xiaonian Li,Zhengbin Zhang,Jianguo Wang
The exploration of efficient and environmentally friendly oxidation method is highly desirable to overcome the critical problems of poor selectivity and heavy metal contamination for the fine chemicals industry. Herein, a self-supported three-dimensional (3D) Se Ni 5 P 4 nanosheet electrocatalyst was rationally designed and fabricated. Benefiting from the synergistic effect of aminoxyl radical and mesoporous Se Ni 5 P 4 /graphite felt (GF), an excellent performance of ≥98% selectivity and 33.12 kg (m −3 h −1 ) space–time yield was obtained for sterol intermediate oxidation with the enhanced mass transfer effect of the continuous flow system. The doping of anionic selenium and phosphorus modulated the electronic structure of Se Ni 5 P 4 , and the oxyhydroxides generated by surface reconstruction accelerated the turnover of 2,2,6,6-tetramethyl-1-piperidine N -oxyl (TEMPO), thereby enhancing the intrinsic electrocatalytic activity. A scale-up experiment was conducted with stacked-flow electrolyzer demonstrated the application potential. This work provided an efficient synergistic electrocatalytic strategy to facilitate rapid electron and mass transfer for electrochemical alcohol oxidation and highlighted the potential for practical electrosynthesis applications.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 13
·2106863
·
IF 15.153
Jie Huang,Yeqing Chen,Pengpeng Rao,Zongming Ni,Xueying Chen,Jie Zhu,Chen Li,Gaoyang Xiong,Ping Liang,Xin He,Songnan Qu,Jun Lin
Carbonized polymer dots (CPDs) have received tremendous attention during the last decade due to their excellent fluorescent properties and catalytic performance. Doping CPDs with transition metal atoms accelerates the local electron flow in CPDs and improves the fluorescent properties and catalytic performance of the CPDs. However, the binding sites and the formation mechanisms of the transition-metal-atom-doped CPDs remain inconclusive. In this work, Mn 2+ -ion–doped CPDs (Mn-CPDs) are synthesized by the hydrothermal method. The Mn 2+ ions form Mn O bonds that bridge the sp 2 domains of carbon cores and increases the effective sp 2 domains in the Mn-CPDs, which redshifts the fluorescence emission peak of the Mn-CPDs slightly. The Mn 2+ ions form covalent bonds in the CPDs and remedy the oxygen vacancies of the CPDs, which cuts off the non-radiative–recombination process of the Mn-CPDs and increases the quantum yield of the Mn-CPDs to 70%. Furthermore, the Mn O bonds accelerate the electron flow between adjacent sp 2 domains and enhances the electron transport in the Mn-CPDs. Thus, the Mn-CPDs demonstrate excellent catalytic performance to activate hydrogen peroxide (H 2 O 2 ) and produce hydroxyl radicals (•OH) to degrade methylene blue (MB) and rhodamine B (RhB).
研究领域:
材料科学
·
纳米技术
·
催化
·
光化学
✓ 已验证
DOI
高影响因子
JOURNAL OF FOOD ENGINEERING
·
2024
·
IF 5.3
Pengkai Xie,Mingcui Huang,Jia Liu,Abdelaziz Elbarbary,Qingzhe Jin,Xingguo Wang,Jun Jin
Poor whipping capabilities of anhydrous milkfat based aerated emulsions pose a fresh challenge to food industrial production, limiting their potential applications in tea drinks, coffee, cakes, and desserts. In this study, the effects of high melting- and low melting-Spans on whipping compatibilities of the aerated emulsions were investigated from view of fat crystal-membrane interactions. With an increase in Spans concentration, there was a corresponding decrease in both fat globule size and interfacial protein. However, in comparison with low melting-Span 20 and Span 80, Span 40 and Span 60 with higher melting points have been found to improve anhydrous milkfat crystal matrix in terms of dense (D f > 1.8) and spot-like crystals (5–10 μm). The interfacial film strength was reduced in this case as both long chain-saturated Spans competitively absorb at the membrane, and elasticity-dominant interfacial membrane was further obtained as their crystallization effects. Occurrence and development of partial coalescence of fat globules (>80% at more than 0.5% addition) were therefore promoted with such fat crystal-membrane interactions during whipping, contributing to a significant improvement in whipping capabilities and heat-stable stabilities of foam structures. A mechanism on the effects of Spans on improving whipping capabilities of aerated emulsions was therefore proposed based on the fat crystal-membrane interactions, which will provide guidance to produce high-quality whipped structures for aerated emulsions.
研究领域:
食品科学
·
胶体化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinyu Zhai,Chunchen Ruan,Lei Chen,Xiaotian Peng,Shuai Yin,Hao Peng
The binary alkane system (C 6 -C 7 , C 6 -C 8 ) was comprehensively explored in this study, and the best cryogenic eutectic n-alkane (70 %C 6 -30 %C 7 ) with freezing point of −115.8℃ and phase transition enthalpy of 123 J/g was designed. After comparing various non-ionic emulsifiers (Span 80, Tween 80, PVA 1788, Arabic gum, Xanthan gum) through volatilization test, Span 80 was selected as the best anti-volatilization emulsifier to synthesize MEPCMs. Different anionic and nonionic emulsifier ratios were studied and determined to be 9:1. Cryogenic MEPCMs were prepared by in-situ polymerization, and the energy storage, thermodynamic, anti-volatilization properties, anti-leakage, mechanical property and durability were characterized. The results show that the morphology of MEPCMs is complete, the core wall materials are well bonded, and the coating rate is 50.9 %. PEG was used as a cross-linking agent to modify the shell of MEPCMs. The characterization results show that PEG effectively improvs the flexibility of the wall material, and the enthalpy loss of the MEPCMs in the anti-leakage test is reduced from 66.4 J/g to 15.8 J/g. The preferred anti-volatilization emulsifier increases the durability of MEPCMs from 192 h to 240 h. After 60 phase transition cycles, the enthalpy value of the MEPCMs is almost unchanged. This study bridges the volatility defects of cryogenic phase change materials and strengthens the durability of MEPCMs in terms of both core-wall and wall materials, which provides an important basis for the utilization of cold energy in cryogenic systems such as LNG, liquid hydrogen, and liquid air.
研究领域:
材料科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Guo Liu,Shan Huang,Xiaochen Liu,Wanzhen Chen,Xin Ma,Shuang Cao,Liping Wang,Lanlan Chen,Huanghao Yang
Transmembrane signal transduction is of profound significance in many biological processes. The dimerization of cell-surface receptors is one prominent mechanism by which signals are transmitted across the membrane and trigger intracellular cascade amplification reactions. Recreating such processes in artificial systems has potential applications in sensing, drug delivery, bioengineering, and providing a new route for a deep understanding of fundamental biological processes. However, it remains a challenge to design artificial signal transduction systems working by the receptor dimerization mechanism in a predictable and smart manner. Here, benefitting from DNA with features of programmability, controllability, and flexible design, we use DNA as a building material to construct an artificial system mimicking dimerization of receptors for signal transduction and cascade amplification. DNA-based membrane-spanning receptor analogues are designed to recognize external signals, which drives two receptors into close spatial proximity to activate DNAzymes inside the cell-mimicking system. The activation of the DNAzyme initiates the catalyzed cleavage of encapsulated substrates and leads to the release of fluorescent second messengers for signal amplification. Such an artificial signal transduction system extends the range of biomimetic DNA-based signaling systems, providing a new avenue to study natural cell signaling processes and artificially regulate biological processes.
研究领域:
合成生物学
·
分子生物学
·
纳米生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 35
·期 2
·e6104
·
IF 3.14
Kuan Wang,Jie Lan,Zhen-Hong He,Zhe Cao,Weitao Wang,Yang Yang,Zhao-Tie Liu
The synthesis of benzyl alcohols (BAs) is highly vital for their wide applications in organic synthesis and pharmaceuticals. Herein, BAs was efficiently synthesized via hydroxymethylation of phenylboronic acids (PBAs) and paraformaldehyde over a simple Rh PPh 3 catalyst combined with an inorganic base (NaOH). A variety of BAs with the groups of CH 3 − , CH 3 O − , Cl − , Br − , and so on were obtained with moderate to good yields, indicating that the protocol had a good universality. Density functional theory (DFT) calculations proposed the Hayashi-type arylation mechanism involved the arylation step of PBA and Rh(OH)(PPh 3 ) 2 catalyst to form Rh(I)-bound aryl intermediates and the hydrolysis step of Rh(I)-bound aryl intermediates and HCHO to generate BA product (the rate-determining step). The present route provides a valuable and direct method for the synthesis of BAs and expands the application range of paraformaldehyde.
研究领域:
有机化学
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE
·
2018
·Vol. 215
·期 11
·1700905
·
IF 1.795
Shuping Deng,Decong Li,Liping Zheng,Yu Tang,Zhong Chen,Luqi Sun,Wenting Liu,Lanxian Shen,Shukang Deng
In this work, the effect of Cd and Sn atoms partly substitution for Zn on among crystal growth, thermal stability, mechanical, and electrical transport property in β-Zn 4 Sb 3 is reported. In a series of samples prepared from the atomic ratios of Zn:Sb:Cd:Sn = 4.4:3: x :3 ( x = 0.2, 0.4, 0.6, and 0.8). Carrier concentration of all samples varies from 4.52 × 10 19 to 6.42 × 10 19 cm −3 as carrier mobility changes from 58.27 to 67.93 cm 2 V −1 s −1 at room temperature. As a result, electrical transport properties of the samples are optimized by Cd Sn co-doped. The experimental density of all the samples varies from 6.26 × 10 3 to 6.34 × 10 3 kg m −3 consistent with the theoretical value. The weight loss and melting point of the sample are determined to discuss thermal stability in the heating process in air, indicating that the single crystals β-Zn 4 Sb 3 possess an excellent thermal stability and it is practical importance in the TE application at high temperature. Consequently, the maximal power factor of 1.70 × 10 −3 W m −1 K −2 is achieved at 540 K for the sample with initial Cd content x = 0.2, which is enhanced by 40% compared with the single-doping system in β-Zn 4 Sb 3 .
研究领域:
材料科学
·
热电材料
·
固体物理
·
无机化学
·
功能材料
✓ 已验证
DOI
高影响因子
Small
·
2017
·Vol. 13
·期 32
·1700805
·
IF 8.643
Wenbo Lu,Tingting Liu,Lisi Xie,Chun Tang,Danni Liu,Shuai Hao,Fengli Qu,Gu Du,Yongjun Ma,Abdullah M. Asiri,Xuping Sun
The development of efficient bifunctional catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of extreme importance for future renewable energy systems. This Communication reports the recent finding that room-temperature treatment of CoO nanowire array on Ti mesh by NaBH 4 in alkaline media leads to in situ development of Co B nanoparticles on nanowire surface. The resulting self-supported Co B@CoO nanoarray behaves as a 3D bifunctional electrocatalyst with high activity and durability for both HER (<17% current density degradation after 20 h electrolysis) and OER (<14% current density degradation after 20 h electrolysis) with the need of the overpotentials of 102 and 290 mV to drive 50 mA cm −2 in 1.0 m KOH, respectively. Moreover, its two-electrode alkaline water electrolyzer also shows remarkably high durability and only demands a cell voltage of 1.67 V to deliver 50 mA cm −2 water-splitting current with a current density retention of 81% after 20 h electrolysis. This work provides a promising methodology for the designing and fabricating of metal-boride based nanoarray as a high-active water-splitting catalyst electrode for applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Simin Yang,Jianqiang Wang,Lifeng Fang,Haibo Lin,Fu Liu,Chuyang Y. Tang
Intercalated structure and electrosprayed interfacial polymerization methods have recently been proposed for permeability enhancement of polyamide membranes. In this study, a Span 80 intercalated polyamide nanofiltration membrane was fabricated through electrospray for simultaneously improving the surface structure, interfacial stability and separation performance. The membrane obtained through electrosprayed interfacial polymerization (EIP) showed a water flux of 83.0 L m -2 h -1 at an applied pressure of 5.0 bar. The intercalated Span 80 severed as multifunctional layer for simultaneously lowering surface roughness (RSa value of polyamide, 7 nm), enhancing interfacial stability (better anti-backwashing ability) and separation performance (enhanced water flux and BPA rejection). The current study provides new opportunities for fabricating polyamide nanofiltration membrane with high performance by combination of EIP and reactive interlayer strategy.
研究领域:
材料科学
·
环境工程
✓ 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）