ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Xiaofei Lei,Xuan Xie,Kanjun Sun,Sitong Liu,Tianyu Hou,Hui Peng,Guofu Ma
Transition metal selenides embedded into a nitrogen, sulfur co-doped carbon materials (TMS@NSC) are promising electrocatalysts to effectively address the sluggish kinetics of oxygen evolution reaction (OER). However, the OER catalytic activity of single metal TMS@NSC is still limited by insufficient active sites. Hence, FeSe 2 and CoSe 2 nanoparticles self-generated and confined in N, S-doped porous carbon (FeSe 2 /CoSe 2 @NSC) catalyst has been synthesized by in-situ polymerization and the subsequent low temperature selenization strategy, aiming to increase the active sites of TMS@NSC. The hybridized FeSe 2 /CoSe 2 @NSC catalyst has excellent OER catalytic activity and good durability in alkaline media, which only requiring an overpotential as low as 278 mV to drive a current density of 10 mA cm −2 , outperforming most recently reported selenide catalysts and commercial RuO 2 catalysts. The high catalytic activity of FeSe 2 /CoSe 2 @NSC catalyst is attributed to the rapid electron transfer between FeSe 2 and CoSe 2 in the unique N, S-doped graphene nanosheets, which effectively inhibits the aggregation of nanoparticles, fully exposes the active sites and provides pathway for oxygen release during the OER process. Moreover, the overall water splitting device assembled with FeSe 2 /CoSe 2 @NSC catalyst showed low overpotential of 1.57 V. This study provides a feasible strategy for the design of high active and stable TMS@NSC catalysts for OER and other energy conversion applications.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Zang Shuaipu,Zhang Xuhui,Sun Yingying,Li Ning,Wang Lei,Li Lin Song
Harnessing environment-friendly and low-cost multinary Cu-In-Zn-S quantum dots (QDs) as emitters for light-emitting diodes (LEDs) has attracted great attention for display and lighting application. However, suboptimal QD structure is a huge obstacle, which results in serious non-radiative recombination and efficiency roll-off. Herein, we synthesized structure-tailored Cu-In-Zn-S/ZnS//ZnS QDs by improving the reactivity of shell growth by 2-ethylhexanoic acid (EHA) ligands. The EHA-assisted shell growth can boost an extended alloyed layer at the core-shell interface and a smoothed confinement barrier, which effectively passivate the interface defects and suppress Förster resonance energy transfer (FRET) process. These synthesized QDs display a bright photoluminescence emission (quantum yield of 83%) and a larger size of 8.4 nm. Moreover, the resulting LEDs based on the EHA-assisted QDs exhibit a maximum luminance of 8074 cd/m2, and a current efficiency of 7.3 cd/A with a low efficiency roll-off. Our results highlight a remarkable ligand strategy to tailor the QD structure for high performance QD-based LEDs.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
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IF 6.371
Xiaofei Fu,Junwu Tao,Zuming He,Yong Gao,Yongmei Xia,Zizhou Zhao
High-efficiency interfacial charge transfer is the key to achieve better spatial carrier separation, and thus to develop advanced heterogeneous photocatalysts for environmental remediation. However, It still remains a great challenge to design and exploit the effective charge transfer scheme. Herein, a novel Z-scheme In 2 S 3 /BiOBr with S−O covalent bonding was prepared by hydrothermal and subsequent thermal annealing methods. The obtained photocatalysts were systematically characterized and used for tetracycline hydrochloride degradation and Cr(VI) reduction in aqueous solution. As a result, the optimized In 2 S 3 /BiOBr heterostructure (IS/BOB-39) exhibited superior photocatalytic activities for tetracycline hydrochloride degradation and Cr(VI) reduction under simulated solar light irradiation compared with individual materials. The Z-scheme transfer mechanism was corroborated by trapping experiments, ESR and XPS analysis , which provided an effective transfer pathway for spatial separation of carriers. Moreover, the formation of chemical S−O bond between In 2 S 3 and BiOBr, which acted as a specific bridge to expediently transmit interfacial electrons, showed a synergistic effect with Z-scheme transfer model on the significantly enhanced photocatalytic performance. In addition, the In 2 S 3 /BiOBr heterojunction presented excellent cycle stability, resulting from the tight heterointerface. This work provides a promising approach to design and fabricate high effect Z-scheme heterojunction in wastewater treatment.
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Solar RRL
·
2022
·Vol. 6
·期 8
·2200150
·
IF 9.173
Chengfeng Ma,Chunxu Xiang,Xinge Liu,Bingyan Li,Xinyu Li,Shuaiqi Han,Qi Dai,Weibo Yan,Hao Xin
Solution-processed chalcopyrite copper indium gallium sulfoselenide (Cu(In,Ga)(S,Se) 2 , CIGSSe) thin-film solar cells have achieved efficiency beyond 18% and have great potential as an alternative to vacuum-based ones. However, most of the efficient solution-based CIGSSe solar cells are fabricated by spin-coating in an inert atmosphere, which limits the transfer from lab protocol to industrial large-scale production. Herein, a scalable doctor-blading technique is applied to fabricate CuIn(S,Se) 2 (CISSe) absorbers from N,N-dimethylformamide molecular precursor solution in ambient air. With the optimization of the precursor concentration to reduce the residue solvent and change the thermal annealing process from one-step to two-step to separate solvent evaporation and complex decomposition to suppress fluidity, high-quality absorber films with densely packed large grains have been fabricated and a champion CISSe solar cell with a power conversion efficiency of 12.54% has been achieved. Importantly, unlike the spin-coating technique which may cause composition change due to the different solubilities of the precursors, the doctor-bladed film has a composition very close to the precursor solution, which is very important for precise control of the absorber composition for industrial production.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Kunyu Chen,Zhanguo Cui,Zhiqiang Zhang,Heliang Pang,Jing Yang,Xiaojiang Huang,Jinsuo Lu
The present study developed a prolonged oxidizable sulfur(IV)/ferrate(VI) system for the generation of hydroxyl radical ( OH) and sulfate radical (SO 4 − ) within 120 min, and proposed a reaction mechanism. In the presence of H + in solution, the S(IV)/Fe(IV) system provided excellent oxidation performance of refractory organics O,O-dimethyl-S-methylcarbamoyl methyl phosphorothioate (dimethoate, a widely used organophosphorus pesticide) within 120 min. The degradation efficiency of dimethoate in the bisulfite/Fe(VI) system (e.g., 90.06% dimethoate) was higher than that in the sulfite/Fe(VI) system (e.g., 51.03% dimethoate), while Fe(VI) alone degraded 27.81% of dimethoate. In the S(IV)/Fe(VI) system, the active species consisted of Fe(VI) (including the highly-reactive iron-based intermediate species, i.e. Fe(V) and Fe(IV)), OH and SO 4 − , with OH being identified as the main active species, contributing more than half of the total. The degradation mechanism of dimethoate in the S(IV)/Fe(VI) system mainly included the cleavage of the S-P bond, C-S bond and the oxidation of the P = S bond. Two plausible degradation pathways were proposed based on the detected transformation products. Dimethoate could be efficiently degraded when the [bisulfite]/[Fe(VI)] molar ratio was 4:1 with a low Fe(VI) dosage (218 µM), the changes in HA and HCO 3 − concentrations affected the transformation of dimethoate, the presence of Cl − , SO 4 2− and NO 3 − had a negligible effect, and the S(IV)/Fe(VI) system performed well in real waters. The S(IV)/Fe(VI) system has excellent oxidation performance for the removal of organic pollutants in water, with a final pH (pH = 6.6) close to neutral and ultimate products of SO 4 2− and Fe(OH) 3 , which has great potential for engineering applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Haoxiang Zhong,Lingzhi Zhang
The low sulfur utilization and the serious shuttle effect of polysulfides severely hamper practical application of Li-S batteries. Herein, sulfur cathodes with the multi-functional structures, featured with double-layered hollow carbon sphere with up to 50 nm interlayer space (DLHC-50) in situ grown Co-SnS catalytic layer is designed and synthesized for lithium sulfur batteries. Co-SnS/DLHC-50 can encapsulate 72% sulfur, higher than 63% for Co-SnS/DLHC-20 due to the large interlayer spaces of DLHC-50. Meanwhile, polysulfides are also effectively restricted via physical entrapment from DLHC-50 as well as chemical binding between Co-SnS and polysulfides. Benefiting from the well-constructed host framework, Co-SnS/DLHC-50 @S shows higher specific capacity/capacity retention of 760.4 mA h g −1 /72.9% after 500 cycles at 0.5 C, than that of 546.5 mA h g −1 /62.2% and 668.9 mA h g −1 /62.2%, for DLHC-50 @S, and Co-SnS/DLHC-20 @S, respectively. In addition, the strategy can be also extended to prepare other metal oxides (sulfides)/DLHC-50 for wide applications. Therefore, this work demonstrates a promising route to combat some bottlenecks such as low sulfur utilization, and the shuttle effect of polysulfides for Li-S batteries.
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CHINESE JOURNAL OF CATALYSIS
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2022
·
IF 12.92
Hui Yang,Jin feng Zhang,Kai Dai
Achieving a strong redox ability and high visible-light absorption ability in a single semiconductor material is difficult. Designing a heterojunction between two semiconductor materials is a feasible method. The new step (S-scheme) heterojunction can effectively promote the separation and transfer of photogenerated electron-hole pairs and retain strong redox ability. We designed and prepared a CdSe 0.8 S 0.2 -diethylenetriamine (DETA)/SnNb 2 O 6 heterostructure material via the solvothermal method. When CdSe 0.8 S 0.2 -DETA and SnNb2O6 form an S-scheme heterojunction, 30%CdSe 0.8 S 0.2 -DETA/SnNb2O6 exhibits the highest CO production rate (17.31 μmol·g –1 ·h –1 ), which is factors of 2.8 and 4.8 higher than that of traditional solvothermal SnNb 2 O 6 (6.2 μmol·g –1 ·h –1 ) and CdSe 0.8 S 0.2 -DETA (3.6 μmol·g –1 ·h –1 ), respectively. X-ray photoelectron spectroscopy characterization data provided evidence that the transfer pathway of space charge in the CO 2 reduction process was in accordance with the S-scheme. This research provides a simple strategy through which one can optimize the band structure to promote the separation of photogenerated carriers and achieve a high efficiency of CO 2 reduction.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Yabin Li,Jingyao Qi,Jimin Shen,Binyuan Wang,Jing Kang,Pengwei Yan,Yizhen Cheng,Li Li,Linlu Shen,Zhonglin Chen
Extensive studies revealed that Cl - could inhibit the removal of targeted pollutants under low Cl - conditions in the peroxymonosulfate (PMS) system. However, the enhanced effect of Cl - has always been overlooked under high Cl - conditions. Here, we find that high concentration of Cl - played a critical role in bisphenol S (BPS) degradation by activating PMS using 16%-CoFe 2 O 4 @PAL (16% [email protected] ). The removal of BPS was sharply enhanced after introducing 0.5 and 1.0 M Cl - , and the corresponding k obs increased to 0.922 min −1 and 1.103 min −1 , which was 6-fold and 7-fold higher than the control (0.144 min −1 ), respectively. HOCl was demonstrated as the dominant species for removing BPS in 16% [email protected] /PMS system under high Cl - circumstances. The typical chlorinated BPS intermediates were identified, which showed higher eco-toxicity than BPS. The chlorinated byproducts along with their toxicity could be effectively eliminated after 30 min. The possible formation mechanism of chlorinated products was further revealed by theoretical calculations. Toxicity assessment experiments showed that BPS significantly affected hormone levels of zebrafish and showed toxicity on the testis and liver of zebrafish, which could be reduced using 16% [email protected] /PMS system. This study attracts attention to the overlooked HOCl in PMS-based processes under high salinity conditions.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Mengna Li,Weiwang Qiu,Qian Wang,Na Li,Lu Liu,Xueli Wang,Jianyong Yu,Xiaoran Li,Faxue Li,Dequn Wu
Bacterial biofilms on wounds can lead to ongoing inflammation and delayed reepithelialization, which brings a heavy burden to the medical systems. Nitric oxide based treatment has attracted attention because it is a promising strategy to eliminate biofilms and heal infected wounds. Herein, a series of tryptophan-based poly(ester urea)s with good biodegradation and biocompatibility were developed for the preparation of composite mats by electrospinning. Furthermore, the mats were grafted with a nitric oxide donor (nitrosoglutathione, GSNO) to provide one type of NO loading cargo. The mats were found to have a prolonged NO release profile for 408 h with a maximum release of 1.0 μmol/L, which had a significant effect on killing bacteria and destructing biofilms. The designed mats were demonstrated to promote the growth of cells, regulate inflammatory factors, and significantly improve collagen deposition in the wound, eventually accelerating wound-size reduction. Thus, the studies presented herein provide insights into the production of NO-releasing wound dressings and support the application of full-thickness wound healing.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qishan Fu,Muzi Yang,Zhongfei Liu,Hao Yang,Fengquan She,Xiaoqi Zhang,Fangyan Xie,Yuwen Hu,Jian Chen
Two-dimensional (2D) transition metal carbides (MXene) have shown great advantages as electrode materials in the new generation of energy storage, especially in supercapacitors . However, the inherent low specific capacitance and restacking layers of nanosheets that occur during electrode preparation further reduce the electrochemical performance of the materials. Based on this, we design a N, S co-doping electrode with a three-dimensional (3D) structure, which not only improves the specific capacitance through fundamentally modifying the electronic structure of the electrode materials, but also effectively improves the rate performance of the electrode by preventing the restacking of 2D materials . The N, S co-doping 3D architecture Ti 3 C 2 T x electrode (TC/NS-3D) exhibits an excellent capacitance value of 440 F g −1 at 5 mV s −1 and 64% capacitance retention rate at a high scan rate of 1000 mV s −1 in 3 mol L −1 H 2 SO 4 electrolyte. The TC/NS-3D electrode also shows excellent capacitance retention of 97.2% after the 10,000 cycles stability test. The density functional theory (DFT) analysis reveals the enhanced performance is attributed to accelerated intermediates transport kinetics promoted by 3D structure engineering and N, S co-doping for Ti 3 C 2 T x . This study is promising in designing heteroatomic doping 3D structure MXene-based materials for electrochemical energy storage systems.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Mingzhu Cui,Zhiqiang Xie,Meiling Wang,Xianming Zhang
Development of a high-performance electrode materials for the simultaneous sensing of ascorbic acid (AA), dopamine (DA) and uric acid (UA) is critical in clinical diagnostics. Novel polymer hydrogel-derived porous carbon has been investigated in sensing due to their high conductivity, hierarchical porous structure and environmental benignity. However, the high cost and cumbersome synthesis of the crosslinker for polymer hydrogel precursors make carbon production by pyrolysis greatly compromised. To address this challenge, here, a facile approach to N, O, S co-doped three-dimensional porous carbon frameworks (N, O, S-HCF) derived from methyl orange (MO) crosslinked polypyrrole hydrogel is developed. Experimental and spectroscopy demonstrate that the derived 3D porous structure and heteroatom doping effect create multidimensional electron transfer pathways and electrocatalytic activity centers. Specifically, the sensor exhibits potent and persistent electrochemical behavior with well-separated oxidation peaks and enhanced oxidation peak currents towards ascorbic acid (AA), dopamine (DA) and uric acid (UA). As a result, the N, O, S-HCF contributes to the effective determination of the three analytes in their mixture and the calibration curves show linear range of 2.5 × 10 −6 –1.0 × 10 −2 M, 1.8 × 10 −7 –8.7 × 10 −5 M, and 2.5 × 10 −7 –1.0 × 10 −4 M with detection limits of 1.0 × 10 −6 , 1.2 × 10 −7 , and 1.8 × 10 −7 M for AA, DA and UA, respectively. This study provides a simple strategy to build heteroatom doped porous carbon for the simultaneous monitoring of multiple electroactive species.
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ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2022
·
IF 3.858
Xiangxiang Wang,Youyu Xie,Zhicai Wang,Ke Zhang,Hualei Wang,Dongzhi Wei
We developed a continuous flow system using ω-transaminase covalently immobilized on an epoxy resin modified with ethylenediamine (EDA) to synthesize (S)-1-Boc-3-aminopiperidine, which is a key intermediate for several novel inhibitors. A second functional group (−NH3+) was introduced to rapidly adsorb ω-transaminase, which was further rigidified by multipoint covalent attachment to the modified resin with high binding efficiency (>95%) and activity recovery (75%). The resulting immobilized ω-transaminase was stable with 90% residual activity after 15 reuse cycles. We synthesized (S)-1-Boc-3-aminopiperidine using this continuous flow system, and 95% conversion was obtained within 10 min of residence. The system was continuously operated for 24 h and achieved a space–time yield of 930.73 g·L–1·day–1, indicating outstanding reaction efficiency. This efficient continuous bioprocess has potential for large-scale production of (S)-1-Boc-3-aminopiperidine.
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