CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Bing Wang,RuiQing Zhang,HuiYong Chen,Zhuo Li,EnZhou Liu,HaiXia Ma,Bo Zhou,Hong Hao,LinYu Jiao
Controllable fine-tuning of heterojunction interfaces at the atomic level represents a promising strategy for enhancing semiconductor photocatalytic performance. Herien, we propose a strategy to introduce hydrogen-bonded electron channels at the heterojunction interface to achieve rapid interfacial electron transfer. This S-scheme hydrogen-bonded supramolecular self-assembled H 12 SubPcB-OPhCH 2 COOH/Ag 3 PO 4 semiconductor heterojunction exhibits efficient and stable photocatalytic degradation of a wide range of pharmaceuticals and personal care products. Experimental results and theoretical simulations demonstrate that the interface O-H⋅⋅⋅O hydrogen bond at the heterojunction generates an internal electric field, which provides the driving force for accelerated S-scheme charge transfer and enhanced redox properties. Furthermore, the combination of TDDFT calculations and synchronous illumination XPS has revealed that hydrogen bonding acts as a suction electron pump in the excited state, transferring electrons from Ag 3 PO 4 to SubPc-2. These findings suggest that hydrogen-bonded supramolecular semiconductor can be used to develop high-performance photocatalytic materials for environmental remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Linfang Cui,Jie Hao,Yan Zhang,Xiaomin Kang,Jiujun Zhang,Xian-Zhu Fu,Jing-Li Luo
Fe-, and N-co-doped carbon (Fe N C) electrocatalysts are promising alternatives to Pt-based catalysts for oxygen reduction reaction (ORR); however, simultaneously enhancing their intrinsic activity and exposure of Fe active sites remains challenging. Herein, we report S-modified Fe single-atom catalysts (SACs) anchored on N,S-co-doped hollow porous nanocarbon (Fe/NS-C) for ORR. The unique hollow structure and large surface area of the SACs are favorable for mass/electron transport and exposure of Fe single-atom active sites. The as-prepared Fe/NS-C electrocatalysts display a high-efficiency ORR activity with a half-wave potential of 0.893 V versus the reversible hydrogen electrode and exceed that of the benchmark commercial Pt/C catalyst as well as most reported transition-metal based SACs. Impressively, the Fe/NS-C-based Al-air battery (AAB) displays a high open circuit voltage of 1.48 V, a maximum power density of 140.16 mW cm −2 , and satisfactory durability, outperforming commercial Pt/C-based AAB. Furthermore, Fe/NS-C exhibits considerable potential as a cathode catalyst for application in direct methanol fuel cells. Experimental and theoretical calculation results reveal that the excellent ORR performance of Fe/NS-C can be contributed to the highly active FeN 3 S sites and the unique hollow structure. This work provides new insights into the rational design and synthesis high-performance ORR electrocatalysts for energy conversion and storage devices. of employing ZIF-8 as precursors.
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高影响因子
Nanoscale
·
2023
·Vol. 15
·期 31
·12961-12971
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IF 6.7
Shuo Wang,Mengke Li,Gaojie Yan,Zhipeng Yang,Yuchao Guo,Xi Sun,Yue Wang,Yi Feng,Huili Ding,Xiaojie Zhang
Lithium–sulfur (Li–S) batteries are severely restricted for practical application due to the polysulfide shuttle effect, Li dendrites and thermal runaway. The use of PEO-based polymer composite electrolytes (PCEs) as an alternative strategy suffers from limited lithium-ion conductivity with deficient long-range transfer route. Herein, Li6.4La3Zr1.4Ta0.6O12 (LLZTO) nanoparticles modified with an in situ-synthesized zwitterionic covalent organic framework layer (denoted as LLZTO@HUT4) were introduced into PEO-based PCEs. Zwitterionic HUT4 modified the lithiophobic LiOH/Li2CO3 layer on the surface of LLZTO nanoparticles, which could notably promote Li+ ion transport for superior electrochemical performance of PCEs. Additionally, the intermediate layer HUT4 located between LLZTO and PEO could further improve the mechanical properties of electrolytes due to the enhanced inorganic/organic interface compatibility and intermolecular interaction. As a result, the obtained LLZTO@HUT4-15%/PEO electrolyte exhibited a competent ionic conductivity of 0.73 mS cm−1 with a Li+ transference number of up to 0.74 at 60 °C. The assembled S@CNT|LLZTO@HUT4-15%/PEO|Li coin cell delivered a considerable initial discharge capacity of 1018 mA h g−1 at 0.2 C, with approximately 92.1% capacity retention after 100 cycles, elucidating an obviously suppressed shuttle effect.
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高影响因子
Solar RRL
·
2023
·Vol. 7
·期 17
·2300318
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IF 7.9
Bowen Liu,Xinan Shi,Wei Shao,Jiaxin Gao,Chenxi Zhao,Fuyan Chen,Dongdong Shen,Bingsuo Zou,Daocheng Pan
Cu(In,Ga)(S,Se) 2 (CIGSSe) solar cells are one of the most promising thin film photovoltaics with a record efficiency of 23.6%. However, the biggest drawback to CIGSSe solar cells is their high material cost, partially resulting from relatively rare and expensive indium and gallium. Therefore, improving the utilization of indium and gallium and reducing their wastage can greatly lower the cost of CIGSSe thin film solar cells. Inkjet printing is a facile, cost-effective, and low-waste deposition technology, which is particularly suitable for low-cost and large-area fabrication of CIGSSe solar cells. Herein, a novel and green ionic liquid-assisted ink to fabricate highly efficient CIGSSe solar cells is developed. The material utilization of inkjet printing can be remarkably improved compared to the conventional vacuum-based deposition approach and spin-coating solution approach. The CIGS printable ink is prepared by dissolving copper acetate, indium acetate, gallium nitrate, and thiourea into ethanol with the assistance of n -butylammonium butyrate ionic liquid. Ionic liquid-assisted CIGS ink has a nearly zero wetting angle and a tunable viscosity, which enable to deposit a flat and continuous CIGS thin film by an inkjet printing method. An encouraging power conversion efficiency of 15.22% has been achieved for inkjet-printed CIGSSe solar cells.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongyu Niu,Xing-Bao Wang,Jingjie Luo,Jiaxin Liu,Chuang Li,Wen-Ying Li,Changhai Liang
Desulfurization plays a critical role in refining crude oil to produce fuel and the manufacture of fine chemicals. However, its low efficiency becomes a great challenge for the present desulfurization if only the C-S cleavage is considered a promising approach to reducing hydrogen consumption under atmospheric pressure. Accordingly, we investigate the critical factors necessary to achieve high C-S cleavage of dibenzothiophenes under mild conditions of 0.1 MPa and H 2 /oil = 100. The mechanism of reactive adsorption desulfurization of dibenzothiophenes with or without steric hindrance at atmospheric pressure on Pt/ZnO is proposed by studying the adsorption model of active metal sites, the Pt efficiency in C-S cleavage influenced by the steric hindrance and the structural evolution of Pt active centers in the presence of sulfur adsorption/deposition. Based on both experimental and DFT results, we report C-S cleavage of dibenzothiophenes with (TOF = 15 h −1 ) or without steric hindrance (TOF = 128 h −1 ) that can be highly efficiently fractured (99.9%) by the interface between PtS x and ZnO . This work has great practical significance for developing atmospheric industrial adsorbents for ultra-deep reactive adsorption desulfurization.
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ENVIRONMENTAL TECHNOLOGY
·
2022
·
IF 3.475
Lu Wang,Yaqun Yu,Guoqiang Liu,Baowei Hu,Junhe Lu
Brominated flame retardants (BFRs) are a group of contaminants of emerging environmental concern. In this study, systematic exploration was carried out to investigate the degradation of tetrabromobisphenol S (TBBPS), a typical emerging BFRs, by thermally activated persulfate (PDS) oxidation. The removal of 5.0 μM TBBPS was 100% after 60 min oxidation treatment under 60°C. Increasing the temperature or initial PDS concentration facilitated the degradation efficiency of TBBPS. The quenching test indicated that TBBPS degradation occurred via the attack of both sulphate radicals and hydroxyl radicals. Natural organic matter (NOM) decreased the removal rate, however, complete disappearance of TBBPS could still be obtained. Six intermediate products were formed during reactions between TBBPS and radicals. Transformation pathways including debromination, β-Scission, and cross-coupling were proposed. Brominated disinfection by-products (DBPs) in situ formed during the degradation of TBBPS were also investigated, such as bromoform and dibromoacetic acid. The presence of NOM reduced the formation rates of brominated DBPs. Results reveal that although thermo-activated PDS is a promising method for TBBPS-contaminated water, it can lead to potential brominated DBPs risks, which should be paid more attention to when SO4•−-based oxidation technology is applied.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2022
·
IF 9.463
Xiaowen Wang,Paul Smith,Zhe Qiang,Qingbao Guan,Zhengwei You,Changhuai Ye,Meifang Zhu
Segregated conductive composites based on all-aromatic liquid crystal polymers (LCPs) are ideal material candidates for electromagnetic interference (EMI) shielding. However, grand challenges still remain for constructing segregated LCP composites due to the sharp viscosity decrease at crystal-to-nematic transition temperature and the very low melt-viscosity of LCPs. Herein, conductive composites based on all-aromatic multiblock poly(esterimide)s (BPEI) and multilayer graphene (MLG) with well-defined segregated structure were fabricated by solid-state compression molding with a broad processing window, which was enabled by the appropriate viscosity at the rubbery state originating from the two very distinct glass transition temperatures of the as-synthesized BPEI block copolymer . The segregated BPEI/MLG composite with 5.0 wt% MLG loading achieves an ultrahigh electrical conductivity of 313.5 S/m and a high EMI shielding effectiveness of 62.2 dB at a thickness of only 2.3 mm. Moreover, the segregated BPEI/MLG composites exhibit high thermal stability and outstanding flame retardancy.
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JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 41
·19431-19446
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IF 4.682
Wang Shouting,Chen Ye,Zhao Yaling,Wei Gangya,Li Dongliang,Liu Xupo
Oxygen reduction reaction (ORR) is a crucial step for Zn-air batteries (ZABs), which requires low-cost yet efficient catalysts to satisfy the practical application. Heteroatom-doped, especially N, S-doped carbon, has attracted intensive attention as promising ORR catalysts. However, the issues of devitalized micropore channels covered by reaction intermediates and unstable configuration of N, S heteroatoms obtained by post-doping treatment have largely hindered the development of carbon-based catalysts. Herein, mesopore-dominated N, S co-doped hierarchical carbon has been constructed by the hard-soft (SiO 2 –ZnCl 2 ) template strategy based on waste biomass. The optimal catalyst (NSC-PT-0.1) exhibits a mesopore-dominated hierarchical porous structure with high S BET (2357.55 m 2 g −1 ) and N, S content (~ 2.32 at.%), resulting in comparable ORR activity in acid ( E 1/2 = 0.69 V) and alkaline ( E 1/2 = 0.83 V) media to Pt/C. Moreover, different biomass precursors of Carrot, Whorled stonecrop, and Ginkgo leaf have been explored to verify the generality of hard-soft template strategy. When NSC-PT-0.1 is applied as the air electrode, the assembled ZAB exhibits high power density of 155.55 mW cm −2 and long-term cycling stability over 216 h. Therefore, this work provides a versatile hard-soft template strategy to synthesize efficient ORR catalysts for ZABs application through the resource utilization of biomass. Graphical abstract Mesopore-dominated N, S co-doped carbon is synthesized by one-step pyrolysis of waste biomass and SiO 2 –ZnCl 2 hard-soft templates. The optimal catalyst exhibits excellent ORR performances in alkaline and acid media as well as promising Zn-air battery application.
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INTERNATIONAL BIODETERIORATION & BIODEGRADATION
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2022
·
IF 4.907
Long Zhang,Man Song,Zhenbo Mao,Yuan Liu,Feng Li,Jiandong Jiang,Kai Chen
Dichlorprop [( R , S )-2-(2,4-dichlorophenoxy)propanoic acid], a chiral herbicide belonging to phenoxyalkanoic acid herbicides, is extensively used around the world, and is frequently detected in various habitats. Although ( S )-dichlorprop has no herbicidal activity, its toxicity and ecological risk are higher than ( R )-dichlorprop. In our previous studies, the isolated strain Sphingopyxis sp. DBS4 was confirmed to mineralize both ( R )-dichlorprop and ( S )-dichlorprop, but the key genes responsible for the initial degradation of ( R )-/( S )-dichlorprop were still unclear. Here, based on genome sequencing and enzyme purification , a new dioxygenase gene, spoA , responsible for the initial transformation of ( S )-dichlorprop to 2,4-dichlorophenol and pyruvate was cloned from the rac -dichlorprop-utilizing strain of Sphingopyxis sp. DBS4. SpoA, an α -ketoglutarate-dependent dioxygenase, exhibited low amino acid sequence identity to the reported ( S )-dichlorprop-transforming dioxygenase SdpA (34.8%), and showed enantioselective activity toward ( S )-enantiomers of dichlorprop and mecoprop, but no activity toward the corresponding ( R )-enantiomers. The K m value of SpoA for ( S )-dichlorprop was 134.3 μM, and the k cat / K m was determined to be 7.5 × 10 −2 μM −1 s −1 . Molecular docking and site-directed mutagenesis showed that two residues of SdpA, Lys101 and Asp119, are the key sites for the enantioselective transformation of ( S )-dichlorprop. Our study identifies a new dioxygenase for the enantioselective transformation of ( S )-dichlorprop and deepens our understanding of the microbial catabolism of chiral phenoxyalkanoic acid herbicides.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Xiaojuan Feng,Yanlong Shi,Jingmei Liang,Wei Li,Xuyuan Gou
Exploring high activity, stable and low-cost electrocatalysts are of great importance for high-efficient hydrogen production via water splitting. Herein, a cactus-like Fe, P co-doped CoNi-S array was constructed via facile hydrothermal reaction and subsequently sulfuration and phosphorization process. Benefiting from the strong synergistic effects of different components, high conductivity of bimetallic sulfide, 3D cactus-like architecture with rich channels for mass/charge transport, and Fe and P co-doping with electron structure regulation, the as-prepared Fe, P-NiCo 2 S 4 /NF presents superior electrocatalytic activity with low overpotentials of 139 and 290 mV to drive the current density of 10 and 40 mA cm −2 for HER and OER, respectively. Meanwhile, it also manifests the distinguished durability for over 60 h in alkaline media. Notably, when integrating in a two-electrode electrolytic cell with Fe, P-CoNi-S, a reduced operation voltage of 1.55 V is required to reach 10 mA cm −2 , which is superior to precious metal-based Pt/C/NF//RuO 2 /NF counterparts. Impressively, it can also be driven by sustainable solar and thermal energies motivated Stirling engine. This work offers a universal strategy for designing high-activity and durable electrocatalysts by dual doping heteroatoms and synergistic interface engineering.
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LANGMUIR
·
2022
·
IF 4.331
Yirui Zhao,Hang Yang,Hongshun Hao,Fuxiao Zhu,Gongliang Zhang,Jingran Bi,Shuang Yan,Hongman Hou
The removal of organic dyes and pathogenic bacteria from contaminated water remains a significant challenge. In the present study, S-type heterojunction Ag2MoO4/ZnFe2O4 (AMO/ZFO) composite nanofibers were synthesized by electrospinning and co-precipitation and fabricated into photoanodes. It is found that the constructed S-type heterojunction of AMO/ZFO composites effectively inhibits the recombination of photogenerated carriers, in addition to the benefits of more exposed active sites and a greater specific surface area. When several properties are improved, AMO/ZFO composites exhibit excellent photoelectrocatalytic performance. The results demonstrate that under visible light irradiation, the photoelectrocatalytic degradation rate of AMO/ZFO-3 to methylene blue reached 76.2% within 50 min, and the killing rate of Salmonella was 83.6% within 80 min. The enhanced photoelectrocatalytic activity was due to the synergy of both electrochemical and photocatalytic effects. More importantly, after four testing cycles, AMO/ZFO-3 still has a better ability to kill pathogenic bacteria and degrade organic dyes due to its high stability. This work provides a feasible method for oxidizing organic dyes and pathogenic bacteria.
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IONICS
·
2022
·Vol. 28
·期 10
·4685-4695
·
IF 2.961
Wang Jie,Xuan Haicheng,Meng Lingxin,Yang Jiangtao,Yang Jiale,Liang Xiaohong,Li Yuping,Han Peide
The development of low-cost and high-efficiency hydrogen evolution reaction (HER) electrocatalysts has become extremely essential to address global energy issues. Herein, we have fabricated arrays of nitrogen and sulfur co-doped CoMoO 4 ultrathin nanosheets grown on nickel foam (N, S-CoMoO 4 /NF 400 ). The experimental results demonstrate that modulating the electronic structure of CoMoO 4 by co-doping N and S atoms is one of the most powerful methods to boost the performance of HER. N, S-CoMoO 4 /NF 400 displays superior HER activity under alkaline environment, with overpotentials of 58 and 119 mV at 10 and 100 mA cm −2 . The excellent performance of the N, S-CoMoO 4 /NF 400 electrode proves that the N, S co-doping engineering can significantly improve the catalytic activity of transition metal-based oxide HER.
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