ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Lei Xiao,Chaowei Yuan,Peng Chen,Yongyi Liu,Jianping Sheng,Shihan Zhang,Fan Dong,Yanjuan Sun
Due to the intrinsic chemically inert CO2 with the dissociation energy of C═O bond as high as 750 kJ mol–1, low efficiency and selectivity have become the most significant restraints for the practical application of photocatalytic CO2 reduction. Renewing the electronic structure of adsorbed CO2 on the catalyst surface through a rational catalyst design is crucial to achieving performance improvement. Herein, we prepared ZnIn2S4 and Cu-substituted ZnIn2S4 containing both Lewis acid and Lewis base sites as a model system for investigating the activation of CO2 by M–S chemical bonds (M represents a metal site). The Cu–S chemical bond can effectively activate CO2 as a vital electron channel and lower the Gibbs free energy for generating the essential intermediate *COOH. Besides, the Cu0.7-ZnIn2S4 sample displays 74.8% selectivity for reducing CO2 to CO with a rate of 47.2 μmol g–1 h–1, roughly 7.14 times that of ZnIn2S4.
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高影响因子
FUEL
·
2022
·
IF 8.035
Baicheng Feng,Zichen Zhang,Jiaqiang Wang,Donglin Yang,Qun Li,Yaping Liu,Hengjun Gai,Tingting Huang,Hongbing Song
The catalytic hydrogenation of carbon dioxide (CO 2 ) into formic acid is among the most important reactions to alleviate global warming and realize the carbon cycle. How to achieve rapid activation of CO 2 remains a challenge. In this work, we designed two novel hydrophobic poly(ionic liquid)s (PILs) with a good affinity for CO 2 . Since the abundant N atoms in the PILs can anchor palladium (Pd) nanoparticles, the designed catalyst can rapidly activate CO 2 and H 2 simultaneously, thus efficiently catalyzing the hydrogenation of CO 2 to formic acid under mild conditions. Due to the synergy from the bis(trifluoromethanesulfonyl)amide anion ([Tf 2 N − ]) with strong hydrophobicity and CO 2 affinity and trimethylamine (NEt 3 ) as a low dissociation energy alkaline additive, the resultant Pd/PIL-bip-Tf 2 N exhibited the best catalytic performance on the hydrogenation of CO 2 to formic acid. The TOF value reached 1,190 h −1 in the aqueous solution of NEt 3 at 100 °C, 1 h, and a total pressure of 4 MPa. The activation energy and dissociation energy during the catalytic process were calculated by DFT, indicating that the synergistic effect of NEt 3 is better than that of other alkaline additives. In addition, the catalytic activity of the catalyst remained stable after several cycling experiments. Based on the obtained results, we proposed a possible reaction pathway. Therefore, PILs have great potential as catalyst carrier material for CO 2 hydrogenation.
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高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 12
·2079
·
IF 5.719
Dong Li,Fachao Wu,Caiyun Gao,Hongfang Shen,Fei Han,Fenglan Han,Zhanlin Chen
In this work, a highly efficient wide-visible-light-driven photoanode, namely, nitrogen and sulfur co-doped tungsten trioxide (S-N-WO3), was synthesized using tungstic acid (H2WO4) as W source and ammonium sulfide ((NH4)2S), which functioned simultaneously as a sulfur source and as a nitrogen source for the co-doping of nitrogen and sulfur. The EDS and XPS results indicated that the controllable formation of either N-doped WO3(N-WO3) or S-N-WO3by changing the nW:n(NH4)2Sratio below or above 1:5. Both N and S contents increased when increasing the nW:n(NH4)2Sratio from 1:0 to 1:15 and thereafter decreased up to 1:25. The UV-visible diffuse reflectance spectra (DRS) of S-N-WO3exhibited a significant redshift of the absorption edge with new shoulders appearing at 470–650 nm, which became more intense as the nW:n(NH4)2Sratio increased from 1:5 and then decreased up to 1:25, with the maximum at 1:15. The values of nW:n(NH4)2Sratio dependence is consistent with the cases of the S and N contents. This suggests that S and N co-doped into the WO3lattice are responsible for the considerable redshift in the absorption edge, with a new shoulder appearing at 470–650 nm owing to the intrabandgap formation above the valence band (VB) edge and a dopant energy level below the conduction band (CB) of WO3. Therefore, benefiting from the S and N co-doping, the S-N-WO3photoanode generated a photoanodic current under visible light irradiation below 580 nm due to the photoelectrochemical (PEC) water oxidation, compared with pure WO3doing so below 470 nm.Keywords:N, S co-doped;water oxidation;tungsten trioxide;photoanode;photoelectrochemical;water splitting
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PubMed
高影响因子
CARBON
·
2022
·
IF 11.307
Wenjie Wei,Fenghong Lu,Lixiu Cui,Yu Zhang,Yanze Wei,Lingbo Zong
Tuning of the coordination environment of atomically dispersed single atoms (SAs) by heteroatom doping is a promising strategy to boost the electrocatalytic activity for oxygen reduction reaction (ORR). The synergistic effect of dual heteroatom doping provides additional degrees of freedom to achieve higher ORR efficiency through decreased energy barriers of the intermediates in catalytic processes. Herein, Fe–SAs anchored within the N, S co-doped porous nanosized carbonaceous spheres (Fe–SAs@N/S-PCSs) was fabricated through the pyrolysis of anchored heteroatom sources and ferric precursors. Under the low catalyst loading capacity of 0.255 mg cm −2 , the obtained Fe–SAs@N/S-PCSs exhibits exceptionally high performance with ORR onset potential (E onset ) of 1.02 V, and half wave potential (E 1/2 ) of 0.90 V (vs. RHE) in 0.1 M KOH solution, outperforming benchmark Pt/C (E onset = 1.01 V, E 1/2 = 0.86 V). Superior oxygen evolution reaction (OER) activity (450 mV at 10 mA cm −2 ) is also demonstrated, thus displaying outstanding performance for Zn-air battery. The porous structure , rich accessible Fe SAs, and the optimal binding of ORR-related species induced by S doping in carbon matrix generate the excellent ORR activity and durability. This work provides insights into the rational design of cost-effective single atom catalysts (SACs) with impressive electrocatalytic activities for efficient energy conversion applications.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Hao Du,Ningyi Li,Lingxuan Yang,Qiang Li,Guoxiang Yang,Qi Wang
Environmental crisis caused by Cr(VI) pollution has gained remarkable attention. Developing efficient photocatalysts for Cr(VI) remediation remains a great challenge. Herein, the Ag@Ag 3 VO 4 /Ag 3 PMo 12 O 40 (Ag@Ag 3 VO 4 /AgPMo) S-scheme heterojunctions were prepared via the combination of hydrothermal and photodeposition methods for Cr(VI) reduction. The resultant S-scheme heterojunctions were characterized to investigate their morphological, structural, photoelectrochemical and optical properties. The synergy of surface plasmon resonance (SPR) effect of Ag and S-scheme hetero-structure improved their photo(electro)chemical performance. Upon visible light irradiation, the optimized Ag@Ag 3 VO 4 /AgPMo delivered superior photoreduction efficiency (94.8%) of Cr(VI) and stability with a slight loss of the performance (92.8% after 6 cycles). The enhancement of Cr(VI) reduction performance may be ascribed to the extended light absorption range and separation and migration pathway of photo-induced electron-hole pairs confirmed by the proposed photoreduction mechanism. This work not only confirms a highly active catalytic system for the light-driven environmental application, but pave a way for the construction of S-scheme heterojunction photocatalysts.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 28
·13527-13540
·
IF 4.682
Chen Dongli,Zhu Ming,Zhan Wenwei,Long Lei,Yu Lu,Zhu Tao,Kang Peibin,Yang Xiaoping,Sui Gang
Abstract Lithium–sulfur (Li–S) batteries have been considered as a promising substitute for lithium-ion batteries because of their high theoretical specific capacity, low cost, and environmental friendliness. However, the further practical application of Li–S batteries is greatly limited by the intrinsic insulation of sulfur, the shuttle effects of polysulfides and sluggish kinetics of the redox reaction. Herein, a well-designed Fe, N co-doped mesoporous carbon sphere (Fe-N-MCS) was fabricated to modify separator for absorbing and reutilizing polysulfides in high-performance Li–S batteries using cost-effective S cathode. The obtained Fe-N-MCS was not only acted as a physical barrier layer to block polysulfides, but also as trapper to capture and anchor polysulfides due to its highly porous structure and N dopants in the carbon frameworks. Furthermore, the high-conductive Fe-N-MCS barrier layer can facilitate electron and ion transfer to improve the electrochemical reutilization of polysulfide trapped therein, because the Fe-N-MCSs exhibited high catalytic activity for enormously boosting the redox kinetics of polysulfides. In consequence, the Li–S batteries with Fe-N-MCS modified separator exhibited high reversible capacity, superior rate capability and impressively cycling stability. The construction of non-precious metal barrier layer with catalyst activity is a promising pathway for the development of high-energy–density Li–S batteries. Graphical abstract The polysulfides were anchored and reutilized by the Fe-N-MCS layer for high-performance lithium sulfur battery.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Qian Wang,Meiling Ge,Xuan Guo,Zhijun Li,Agen Huang,Fu Yang,Rong Guo
The mesoporous supports of alkylated poly(ionic liquid)s (PILs) are got through free radical copolymerization . With an immobilization yield of 99% for Candida antarctica lipase B (CalB), the biocatalyst showed high advantage for biodiesel production under mild conditions. Typical catalyst CalB 0.2 @PIL-C8 was capable of effectively converting soybean oil into biodiesel with a yield of 68.2%, which is higher than Novozym 435 for 57.5%. The biodiesel yield was almost 1.5 folds compared to that of free CalB under the same conditions. And the catalyst remained about 80% activity in a seven-run recovery test with no CalB leaching in the whole process. The hydrophobic PILs not only provide a suitable reaction micro-environment but also can help CalB keep an open conformation in immobilizing with its flexible hydrophobic alkyl chains. This research offered a green and effective strategy for regulating the hydrophobicity and surface potential of support to enhance the performance of immobilized lipase.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 3
·1977-1993
·
IF 4.682
Weng Peijie,Cai Qing,Wu Huadong,Zhang Linfeng,Wu Kun,Guo Jia
The flower-like CQDs/ S -Bi 4 O 5 Br 2 composites photocatalyst with high visible-light response is prepared by adjusting bismuth-rich, S -doped, and introducing carbon quantum dots (CQDs) into the bismuth oxybromide (BiOBr). Particularly, the prepared C 10 /S 6 –Bi 4 O 5 Br 2 composite shows the highest degradation efficiency for the ciprofloxacin (CIP) under visible-light irradiation with the apparent rate constants k of 0.03798 min −1 , which is 26.3 times and 10.1 times higher than that of BiOBr and Bi 4 O 5 Br 2 , respectively. The sulfur doping leads to the increase of the specific surface area and decreases of the band gap but retains the original flower-like morphology of Bi 4 O 5 Br 2 . Compared to the pure Bi 4 O 5 Br 2 , CQDs/Bi 4 O 5 Br 2 , and S -Bi 4 O 5 Br 2 , the CQDs introduction and S -doping can improve both of the light absorption range and intensity, as well as the charge transfer efficiency for the C 10 /S 6 –Bi 4 O 5 Br 2 composites. Furthermore, because of the combination of the CQDs and S doped for the Bi 4 O 5 Br 2 composites, the separation efficiency of photo-generated carriers is improved with the recombination rate greatly reduced. Graphical Abstract
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yibo Yuan,Xipeng Wei,Hua Yin,Minghan Zhu,Haoyu Luo,Zhi Dang
The effects of organic acids on hexavalent chromium (Cr(VI)) removal by reduced iron-based materials have been extensively studied. Nevertheless, the promotion mechanism from the perspective of the electron transfer process is still unclear. Herein, sulfidated nanoscale zero-valent iron (S-nZVI) and the selected organic acids, citric acid (containing both -OH and −COOH groups) and oxalic acid (containing only −COOH groups), showed significant synergistic promotion effects in Cr(VI) removal. The FeS and FeS 2 on S-nZVI surface could enhance the Cr(VI) reduction as the reductive entity and electron conductor. Furthermore, even though the reactivity of FeS with Cr(VI) is higher than that with FeS 2 , the Cr(VI) removal efficiency by FeS 2 was much higher than that by FeS with organic acids. Under neutral and alkaline conditions (pH 6.0–8.0), organic acids promoted the diffusion, adsorption and complexation of Cr(VI) on S-nZVI surface, thus enhancing the electron selectivity towards Cr(VI). However, when the solution pH changed to acidic conditions (pH 4.0), organic acids facilitated the dissolution of Fe(II) ions from S-nZVI and enhanced the electron utilization towards Cr(VI) via the fast Fe(III) reduction process. This study provided a new insight into the Cr(VI) removal, which was beneficial to understand the application boundaries of S-nZVI for Cr(VI) remediation.
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PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 31
·17694-17708
·
IF 4.22
Bu Jingting,Zhou Zhipeng,Wu Xiaomin,Zhang Chenying,Li Zhen
Biomass-derived carbon materials are often applied in green energy storage systems like supercapacitors due to the abundance, facile access, low cost and nontoxicity. In this work, biomass-derived porous carbon spheres (PCSs) have been prepared by the carbonization and etching of sodium alginate (SA). Using polyacrylic acid (PAA) as a template, N-doped graphene quantum dots (N-GQDs) are grown evenly on the surface of the PCSs, which drastically improves the pseudocapacitive activity and electrical conductivity. The prepared N-GQD/PCS/PAA electrode has a remarkable specific capacitance of 419.3 F g −1 at 1 A g −1 . The symmetric supercapacitor assembled with N-GQD/PCS/PAA electrode exhibits a great specific capacitance of 337.5 F g −1 at 0.5 A g −1 . Particularly, the device displays an ultrafast charge/discharge rate of 2.5 V s −1 , demonstrating excellent rate capability and structural stability. The supercapacitor based on N-GQD/PCS/PAA possesses high energy density of 11.72 W h kg −1 and excellent cycle stability. A high mass loading (9.18 mg cm −2 ) with the energy density of 8.54 W h kg −1 is also investigated to realize the practical application for the device. In general, a novel biomass-derived carbon electrode modified with highly electrochemical active N-doped graphene quantum dots has been constructed to provide an effective way for high performance energy storage.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Jianwei Liu,Jianan Wang,Lei Zhu,Xin Chen,Qianyue Ma,Zhicheng Xu,Shiyi Sun,Ning Wang,Qinqin Chai,Wei Yan
Lithium-sulfur (Li-S) batteries are considered to be promising candidates for next-generation storage systems. However, the practical applications are still hindered by the severe capacity decay, mainly caused by the large volume change, polysulfide shuttle and sluggish sulfur conversion kinetics. Herein, hollow urchin-like Mn 3 O 4 (HU-Mn 3 O 4 ) microspheres as sulfur hosts have been synthesized by the hydrothermal method and calcination treatment, aiming to prevent the polysulfide dissolution (benefiting from the strong polysulfide anchoring effect of Mn 3 O 4 ) and alleviate the volume expansion of sulfur (benefiting from the special hollow structure). Meanwhile, the urchin-like thorny surface also facilitates the rapid ion/electron transfer and the abundant active sites for the fast sulfur redox kinetics. When used as the sulfur host in Li-S batteries, the S@HU-Mn 3 O 4 cathode delivers a high initial capacity of 1137.4 mAh g −1 with a slow capacity decay of 0.042% after 200 cycles at 0.2 C. Even under the conditions of lean electrolyte (E/S = 7 mL g −1 ) and low N/P ratio (N/P = 2.1), the S@HU-Mn 3 O 4 cathode still enables a stable cycling performance with a high gravimetric energy density (202 Wh kg cell −1 ), demonstrating its great potential in the development of future practical Li-S battery materials.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mei Zhang,You Xu,Hugang Zhang,Zhongyao Duan,Tianlun Ren,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Pd-based materials are promising alternatives to Pt for oxygen reduction reactions (ORR), which is the critical electrode reaction for many oxygen-electrocatalysis-based energy storage and conversion devices. Modification of electronic structure and support effect are powerful tools for boosting ORR performance of Pd-based catalysts. Herein, phosphorus (P) doped-palladium sulfide (Pd 4 S) nanoparticles decorated on P/sulfur (S) co-doped reduced graphene oxide (P-Pd 4 S/PSG) is prepared via a one-step solvothermal method using triphenylphosphine sulfide as both P and S sources. The incorporation of P effectively tailors the electronic structure and coordination environment of Pd 4 S, while P-Pd 4 S decorated on PSG generates strong metal-support interaction, which synergistically promotes electrocatalytic performance towards ORR. The proposed synthetic method offers a feasible route for the rational construction of heteroatoms-doped carbon − metal composites with high-performance for ORR and other potential energy applications.
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高影响因子
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