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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 33 ·期 3 ·2210551 · IF 19.924

Two-Step Cooling Strategy for Synergistic Control of CuZn and SnZn Defects Enabling 12.87% Efficiency (Ag,Cu)2ZnSn(S,Se)4 Solar Cells

Hang Geng,Mengyang Wang,Songfan Wang,Dongxing Kou,Zhengji Zhou,Wenhui Zhou,Yafang Qi,Shengjie Yuan,Litao Han,Yuena Meng,Sixin Wu

Abundant intrinsic defects and defect clusters in Cu 2 ZnSn(S,Se) 4 (CZTSSe) solar cells lead to severe nonradiative recombination and limited photoelectric performance. Therefore, developing effective method to suppress the detrimental defects is the key to achieve high-efficiency solar cell. Herein, a convenient two-step cooling strategy in selenization process is reported to suppress the Cu Zn and Sn Zn defects and defect clusters synergistically. The results show that rapid cooling during section from selenization temperature to turning temperature can inhibit the volatilization of Sn and restrain the corresponding Sn-related defects, while slow cooling during the subsequent temperature section can reduce the degree of Cu-Zn disorder. Benefitting from the synergistic effect of two-step cooling, a significantly lowered concentration of Sn Zn and Cu Zn defect and their defect clusters [2Cu Zn +Sn Zn ] in absorber is observed, meanwhile, a reduced band tailing effect and promoted carrier collection efficiency of the photovoltaic device is obtained. Finally, a device with improved open-circuit voltage ( V oc ) of 505.5 mV and efficiency of 12.87% is achieved. This study demonstrates the impact of cooling process on defects controlling for the first time and provides a simple and effective new strategy for intrinsic defect control, which may be universal in other inorganic thin film solar cells.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Activating and optimizing the MoS2@MoO3 S-scheme heterojunction catalyst through interface engineering to form a sulfur-rich surface for photocatalyst hydrogen evolution

Lijun Zhang,Zhiliang Jin,Noritatsu Tsubaki

As a crucial part of artificial photosynthesis, the design of the catalyst is important essential. Among them, the interface engineering between semiconductors and the construction of surface-active sites play a vital role in generating and transporting light-excited electrons, which can ultimately accelerate water decomposition. Therefore, the MoS 2 @MoO 3 step (S)-scheme heterojunction photocatalyst was prepared by in-situ partial sulfidation. The excellent interface engineering of MoS 2 @MoO 3 nanomaterials achieves a high surface reaction rate. The in-situ vulcanization strategy gradually corrodes from the outside to the inside. The introduction of sulfur atoms can replace oxygen atoms to build a sulfur-rich surface and generate molybdenum sulfide. The amount of thioacetamide is adjusted to control vulcanization and optimizing the experimental conditions, the best hydrogen production rate is 12416.8 µmol h −1 g −1 . An in-situ irradiation XPS experiments and DFT calculations provide a deeper understanding of the S-scheme electron transport mechanism in MoS 2 @MoO 3 . MoS 2 @MoO 3 interface interaction has penetrating electron channels and a strong interface interaction force, which effectively promotes the charge transfer between interfaces. This gradual surface vulcanization strategy provides new ideas for introducing synergistic surface-active sites and optimizing interface engineering photocatalyst projects.

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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2022 ·Vol. 29 ·期 32 ·48638-48647 · IF 5.19

Simultaneous biodegradation of dimethyl sulfide and 1-propanethiol by Pseudomonas putida S-1 and Alcaligenes sp. SY1: “Lag” cause, reduction, and kinetics exploration

Li Qian,Tang Zeqin,Zhang Jiahui,Hu Jingtao,Chen Jianmeng,Chen Dongzhi

Simultaneous biodegradation of malodorous 1-propanethiol (PT) and dimethyl sulfide (DMS) by Pseudomonas putida S-1 and Alcaligenes sp. SY1 was investigated and the interactions implicated were explored. Results showed that PT was completely degraded in 33 h, while a lag of 10 h was observed for DMS degradation alone, and the lag was even extended to 81 h in the binary mixture. Mechanism analysis found that the lag was mainly attributed to the exposure of DMS degrader ( Alcaligenes sp. SY1), rather than PT metabolites and PT degrader. The exposure time and PT concentration also influenced the lag duration much. Citric acid could effectively reduce the lag. Pseudo-first-order model was proved suitable for the description of PT degradation, revealing that PT degradation could be enhanced in presence of DMS with a concentration of < 50 mg L −1 . A modified Gompertz model, incorporated the lag phase, was developed for the description of DMS degradation in the mixture, revealing that DMS degradation depended on the initial PT concentration, and when the lag was not considered, PT with low-concentration could promote DMS biodegradation, while a higher concentration (> 20 mg L −1 ) cast negative effect.

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RENEWABLE ENERGY · 2022 · IF 8.634

Self-activated pyrolytic synthesis of S, N and O co-doped porous carbon derived from discarded COVID-19 masks for lithium sulfur batteries

Chao Yuwen,Bingguo Liu,Qian Rong,Libo Zhang,Shenghui Guo

The continuous spread of COVID-19 has produced a large number of abandoned disposable medical masks (DMMs), which have a greater negative impact on the environment and biosafety. In response to this issue, a method for rapid microwave sulfonation , nitrification and oxidation of DMMs was proposed to convert DMMs with low carbonization efficiency into aromatic carbon with good thermal stability , which not only maintained 51 wt% of initial mass at 1000 °C, but also achieved in situ co-doping of S, N and O. Subsequently, porous carbons derived from DMMs were synthesized by self-activation pyrolysis , which avoided consumption of alkali and metal salts in the traditional activation process . It was further found that low pyrolysis temperature was not enough to produce enough active material H 2 and H 2 O to obtain high specific surface area, while increasing pyrolysis temperature could adjust the specific surface area of as-prepared carbon, ranging from 52 m 2 ·g −1 to as high as 890 m 2  g −1 . Thanks to synergistic effect of S, N, and O co-doping and hierarchical porous structure , the first discharge specific capacity of sample synthesized by self-activated pyrolysis at 900 °C was 1459.8 mAh·g −1 at 0.1 C, and the discharge specific capacity retention at 0.5 C after 400 cycles was 52.3%.

CAS / MDL: 57-13-6
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Enhanced Shape Memory Metal-Coordinated Poly(aryl ether ketone)s with Tunable Gradient-Deformation Behaviors as well as Self-Healing and Reprocessing Abilities

Shuai Yang,Yang He,Jinsong Leng

Reversible dynamic bonds are able to crack and recombine upon external stimuli, which endow polymers with exceptional self-healing, reprocessing, and reversible deformation ability. In this paper, we integrated the metal coordination bonds into shape memory poly(aryl ether ketone) (PAEK) to fabricate smart materials with multifunctionalities. Through tuning the metal ion content and species, the enhancement of shape memory behaviors was achieved, including the high recovery ratio (over 98%) and fixity ratio (over 98%), which was closely related to the synergic effect of the intrinsic motion ability of PAEK matrix and the cracking-recombination of coordination bonds. Besides, through the combination of the components with different Cu2+ contents, in addition to the components with Fe2+ coordination bonds, we fabricated the gradient shape memory structures with controllable shape memory and recovery behaviors. The manipulation of gradient coordination bonds resulted in different shape recovery speeds and directions. Furthermore, due to the dynamic cracking-recombination of coordination bonds, the metal-coordinated PAEK material exhibited the great self-healing and reprocessing performances, which were significant for largely extending its application range.

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POLYMER · 2022 · IF 4.432

Development of rigid side-chain poly(ether sulfone)s based anion exchange membrane with multiple annular quaternary ammonium ion groups for fuel cells

Shenghua Du,Songsong Li,Ning Xie,Yaoyao Xu,Qiang Weng,Xingming Ning,Pei Chen,Xinbing Chen,Zhongwei An

A variety of poly (ether sulfone)s based anion exchange membranes (AEMs) rPES(x/y)-Q with high-density heterocyclic quaternary ammonium groups is prepared by a polycondensation of novel difluoro monomer with biphenol and bis(4-fluorophenyl) sulfone . The AEMs rPES(x/y)-Q exhibit low IEC values in the range of 0.82–1.33 mequiv. g −1 but relatively high hydroxide conductivity of 54.1–82.3 mS cm −1  at 80 °C. Moreover, the AEMs rPES(x/y)-Q display affordable water uptake and good stability due to their rigid side-chain, high-density and stable heterocyclic quaternary ammonium cations. Noticeably, the rPES(5/20)-MPy based single fuel cell displays a large maximum power density of 141 mW cm −2 , which reveals a potential application in anion exchange membrane fuel cell.

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Materials Today Sustainability · 2022 · IF 7.244

Synergic adsorption and catalytic conversion of polysulfides based on polar Mo2C and pyridinic N for the enhanced electrochemical performance of Li–S batteries

Y. Liu,H. Liu,L. Tian,L. Pang,X. Liu,J. Li

As a most promising potential next-generation energy storage system , lithium-sulfur batteries (Li–S batteries) received great attention in recent years. However, how to effectively prevent the shuttling effect and accelerate the redox reaction kinetics of polysulfides are still a challenge. Herein, a strategy of using the soft template as a pore-forming agent was proposed to prepare Mo 2 C/nitrogen-doped carbon hollow microflowers (marked as H–Mo 2 C/NC MFs), which was used as an efficient absorbent and electrocatalyst of polysulfides for Li–S batteries. Due to the physical limitations of assembling the special nanosheet into a hollow carbon matrix in the shape of a microflower, the H–Mo 2 C/NC MFs can be used as an appropriate S loading substrate. With the synergistic chemisorption from pyridine N sites and high content polar Mo 2 C nanoparticles , the as-prepared H–Mo 2 C/NC MFs can provide enhancing adsorption and catalytic conversion for polysulfides. As a result, the H–Mo 2 C/NC/S MFs-based cathode provides a high initial discharge capacity of 1104.8mAh/g at 0.2C. Even at the high rate of 1.0C, the initial capacity of 705.2mAh/g still shows good electrochemical performance, and in 1000 cycles, the average capacity decay rate is only 0.016%, with supercycle stability. This article provided a new strategy for a novel viewpoint for the reasonable design of conductive and polar materials for efficient and durable Li–S batteries.

CAS / MDL: 62-31-7
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DIAMOND AND RELATED MATERIALS · 2022 · IF 3.806

O3-assisted low-temperature preparation of marginal S and graphitic N co-doped graphene oxide as high-performance electrocatalyst for bisphenol A degradation

Qian Zhang,Si Chen,Zhi Huang,Yanying Liu,Jun-ming Hong

In this research, a novel insight was provided for oriented low-temperature S and N doping into graphene oxide (GO).Given the gradual concern in the high-temperature dependence of traditional annealing method for the oriented design of heteroatom doping, utilizing O 3 etching-assisted heteroatom doping can simultaneously resolve the problems of energy consumption and doping species design. In this research, with O 3 etching, 100 at.% marginal S (C-SO X -C) and 92 at.% graphitic N co-doped O 3 -S/NGO were successfully synthesized at annealing temperature of 200 °C. Characterization results showed that S and N doping via O 3 etching maintained the sheet-like structure of GO without much stacking (layer thickness of 4–5 nm). In addition, active defects were formed by O 3 etching and S/N atom doping to provide active center for catalytic reaction . The electrocatalytic degradation behavior proved that 100 % bisphenol A degradation efficiency could be achieved by O 3 -S/NGO within 30 min and that the main active species generated during the reaction were O 2 •− , 1 O 2 and active chlorine. The possible pathways of bisphenol A degradation were also determined to complete the discussion. This project was based on the environmental demand of organic pollution control and suggested an optimal preparation strategy for high-performance catalyst preparation and utilization.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

From pure water to hydrogen peroxide on a novel 2,5,8-triamino-tri-s-triazine (melem)-derived photocatalyst with a high apparent quantum efficiency

Qiaoyu Zhang,Chengcheng Chen,Fangting Liu,Zhengguo Zhang,Xiaoming Fang

Photocatalytic hydrogen peroxide (H 2 O 2 ) production is a green process but remains a great challenge. Herein, a novel photocatalyst with high activity for H 2 O 2 production, is developed based on 2,5,8-triamino-tri-s-triazine (melem) by linking it with 2, 3-naphthalene dicarboxylic anhydride (NDA). The obtained melem/NDA hybrid not only exhibited narrowed band gap and obviously enhanced visible light absorption, but also showed reduced charge recombination originated from its spatial distribution in HOMO and LUMO induced by the introduction of NDA as verified by DFT calculations. More significantly, the sufficient LUMO and HOMO positions for the optimal sample, melem/NDA 0.5 , ensured efficient H 2 O 2 production from pure water via both the oxygen reduction reactions mainly through the two-step one-electron path and the water oxidation reaction through the one-step two-electron path. Consequently, melem/NDA 0.5 achieves an apparent quantum efficiency of as high as 6.9 % at 420 nm. This work sheds light on developing high-performance organic photocatalysts for boosting photocatalytic H 2 O 2 production.

CAS / MDL: 106-51-4
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Sea-Urchin carbon nitride with carbon vacancies (C-v) and oxygen substitution (O-s) for photodegradation of Tetracycline: Performance, mechanism insight and pathways

Hao Zhang,Yunxiong Zeng,Xinqing Wang,Xingyu Zhan,Jingcai Xu,Ao Jin,Bo Hong

The fast recombination of electron-hole pairs results in low photoactivity, limiting carbon nitride further application in wastewater purification. To address this issue, regulation of electron configuration via optimizing surface atom properties is a promising strategy for improving the separation of electron-hole pairs. Here, sea-urchin carbon nitride (SUCN-6) with C-v and O-s mediated electronic structures were facile prepared, endowing it with a decrease in transportation resistance of charge carriers and increased activation towards oxygen. Under visible light, the SUCN-6 showed a removal efficiency of ∼ 89% towards tetracycline (TC) in 20 min and no obvious decaying after five consecutive cycles. This TC photodegradation follows a first-order kinetic, and its kinetic constant reaches 0.0908 min −1 , which is 2.35 folds higher than that of pristine carbon nitride. In addition, several crucial factors of practical wastewater purification (such as pH, TC concentration, water sources, inorganic salts, and organic matters) that might affect photoactivity were investigated. Moreover, the degradation pathways of TC and intermediates were detected by an HPLC-MS and electron spin resonance instrument, and a possible photodegradation mechanism over SUCN-6 was elucidated. This study offers new insights into the photocatalysis kinetics and photodegradation mechanism over carbon nitride for environmental remediation.

CAS / MDL: 64-75-5
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2022 ·Vol. 414 ·期 24 ·7253-7263 · IF 4.478

Synthesis of intrinsic dual-emission type N,S-doped carbon dots for ratiometric fluorescence detection of Cr (VI) and application in cellular imaging

Mei Xiping,Wang Dongxiu,Wang Songbai,Li Junfen,Dong Chuan

In this paper, intrinsic dual-emission fluorescent carbon dots (CDs) doped with N and S atoms have been firstly fabricated. The characterization results show that CDs are successfully synthesized with two separate fluorescence emissions at 468 nm and 628 nm, respectively. The strong and selective interaction of Cr (VI) ions with CDs lead to obvious fluorescence decrease of CDs at 468 nm, which is caused by a mixed quenching mechanism. At the same time, the fluorescence at 628 nm increase. Interestingly, the CDs solution show obvious color change under the daylight and UV light, so visualization detection of Cr (VI) can be realized in water samples. Based on the data of the emission intensity ratios of F 468 / F 628 , Cr (VI) can be detected from 3.8 to 38.9 μM combined with the linear correlation coefficient of 0.998, and the lowest detection concentration is 47.2 nM. The platform is satisfactorily applied to the detection of Cr (VI) ions in water samples. In addition, the CDs could be applied as fluorescent probes for cell imaging with dual fluorescent emission. Graphical abstract

CAS / MDL: 7647-14-5 7664-93-9
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

Rational introduction of S and P in multi-stage electrocatalyst to drive a large-current-density water oxidation reaction and overall water splitting

Yijie Zhang,Leran Liu,Jinwei Wang,Rui Yao,Yun Wu,Muheng Wang,Qiang Zhao,Jinping Li,Guang Liu

Rational design and construction of electrocatalysts that can work well at large current densities are imperative for water splitting. Herein, a multi-stage P–Ni 3 S 2 /NiFe/NF electrocatalyst was rationally designed by introducing heteroatoms (S and P) and heterostructure construction. Benefitting from the optimized electronic structure configuration by the synergistic incorporation of S and P, the as-prepared P–Ni 3 S 2 /NiFe/NF electrocatalyst exhibits remarkable activity and stability towards oxygen evolution reaction (OER) in alkaline media , yielding ultralow overpotentials of 250 mV and 372 mV at the current densities of 100 mA/cm 2 and 1000 mA/cm 2 , respectively. Moreover, its multi-stage heterostructure also endows the electrocatalyst with unique multifunctional properties, making it can realize overall water splitting under a low cell voltage of 1.57 V at 10 mA/cm 2 , and has long-term stability. This work demonstrates the importance of rational introduction of heteroatoms and interface/surface engineering for advanced electrocatalytic materials.

CAS / MDL: 13472-35-0
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