JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Jingyuan Liu,Min Liu,Subin Zheng,Xiaoyang Liu,Shunyu Yao,Fengyang Jing,Gang Chen
The construction of S-scheme heterojunctions is an effective approach to realize artificial photocatalytic processes. For the higher solar energy conversion efficiency, current research focuses on improving the interfacial intimacy and precisely modulating the strength of the internal electric field (IEF). To address this issue, we propose a novel MOF-based synthesis and derivation strategy. The heterojunction obtained by this strategy tends to form an intimate interface and a tunable IEF, which facilitates the transfer and separation of photogenerated carriers. Herein, a ZnS/ZnIn 2 S 4 (ZIS) S-Scheme heterojunction containing sulfur vacancies (Sv) was successfully synthesized, and its good photocatalytic hydrogen evolution reaction (HER) and CO 2 reduction reaction (CO 2 RR) activity confirmed the feasibility of this strategy. The prepared Sv-ZnS/ZIS exhibits an apparent quantum yield of 19.8 ± 1.0 % at 420 nm and a hydrogen evolution rate of 2912.3 ± 185.9 μmol g −1 h −1 , which is 9.0 and 33.6 times higher than pure ZIS and Sv-ZnS, respectively. Furthermore, the yield of photoreduction CO 2 to CO reaches 2075.7 ± 63.0 μmol g −1 h −1 with a CO selectivity of 93.0 ± 0.8 %. This work provides new sights for the rational design and construction of S-scheme photocatalysts with sulfur vacancies for efficient photocatalysis.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Menglan Gao,Xiaobin Liao,Jing Yu,Xinna Lin,Huan Qi,Linlu Shen,Shupo Liu,Zhimin Yang
Bromide ions (Br - ) affected non-brominated nitroso-dimethylamine (NDMA) formation during ozonation , but the mechanism is still unclear. 1,1,1′,1′-tetramethyl-4,4′-(methylene-di- p -phenylene) di-semicarbazide (TMDS) was chosen to further probe this problem. The results indicated that low levels of Br - (≤20 μM) enhanced NDMA from 3.27 to 7.56 μg/L, while its amount slightly dropped to 6.22 μg/L raising Br - to 100 μM. It was experimentally verified that intermediates 1,1-dimethylsemicarbazide (DMSC) and 1,1-dimethylhydrazine (UDMH) played important roles on promoting NDMA generation, whose contribution rates were 40.2% and 32.2%, respectively. The brominated substances with higher NDMA molar yields were detected. ∙OH reduced NDMA formation without Br - , while it played promotion role with Br - ; the corresponding contribution rates were − 26.9% and 29.2%, respectively. No matter with or without Br - , both ∙O 2 - and l O 2 brought a boost to NDMA formation, their contribution ratios were 34.9% and 58.1% without Br - , while raised significantly to 64.6% and 81.5% when Br - existed. Br - not only facilitated NDMA formation, but also benefited the degradation of TMDS. Based on the calculation results and intermediates detected, the influence mechanisms of Br - were proposed. The results would provide theoretical basis and technical guarantee for treating NDMA precursors and bromide co-existing water in the future.
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Environmental Science-Nano
·
2023
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IF 7.3
Jinli Qiu,Huifang Chan,Wenting Zheng,Yao Feng,Fuqiang Liu
The design of metal–organic framework-derived metal oxides/sulfides is an effective approach for water remediation. A series of Fe–Ce composites (Fe–Ce–S–N) with cluster-like morphology were prepared with prussian blue analogue (PBA) as the precursor in a hydrothermal process. S doping promoted the conversion of Fe(III) to Fe(II), which greatly improved the performance of the Fenton-like reaction. The optimized Fe–Ce–S–N catalyst exhibited superior catalytic activity towards sulfamethoxazole (SMZ) degradation (18.63 mgSMZ gcat−1 min−1), showing the largest k value (0.1862 min−1), which was 2.1 and 8.1 times higher than that of Fe–Ce–S–H and Fe–Ce–N, respectively. Moreover, the Fe–Ce–S–N catalyst displayed a remarkable reusability, stability and adaptability in Fenton-like systems. Overall, this work provides new insights into extending novel PBA-derived catalysts to significantly improve heterogeneous Fenton-like performances.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Ming-Dan Yao,Qi Liu,Zhe Feng,Ji Cai-Rang,Zi-Long Yang,Yu-long Xie
The heterostructure enhances the stability and activity of the catalyst. • The interfacial electron transfer and slight reconstruction synergistically enhance the catalyst performance. • d-p orbital hybridization enhances the metal synergy. • The formation of the heterojunction alters the rate-determining step of the reaction. This paper reports on a Ni 3 S 2 /NiFe-LDH heterostructure grown in-situ on a nickel foam substrate via a one-step hydrothermal method, and systematically evaluates its oxygen evolution reaction performance. This catalyst requires an overpotential of only 284 mV to reach a current density of 300 mA·cm −2 . Benefiting from the construction of the heterointerface, following 100 h galvanostatic electrolysis at 50 mA cm −2 , merely a 12 mV increase in overpotential was detected at 300 mA cm −2 in post-stability LSV tests. In-depth mechanistic analysis reveals that the introduction of Ni 3 S 2 triggers interfacial electronic reconstruction. Spin polarization and orbital hybridization collectively optimize the density of states of NiFe-LDH, accelerate charge transfer, and enhances its intrinsic catalytic kinetics. This work not only develops a high-performance oxygen evolution catalyst, but also provides a rational strategy for modulating electronic structures via heterointerface engineering to enhance electrocatalytic performance. Download: Download high-res image (328KB) Download: Download full-size image
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EUROPEAN POLYMER JOURNAL
·
2023
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IF 6
Pengyun Zhao,Lingxin Meng,Jingmei Xu,Jinxuan Lei,Kuirong Feng,Tian Lan,Zhe Wang
In this study, composite proton exchange membranes (PEMs) based on functional graphene oxide (GO) and carboxyl-containing sulfonated poly(arylene ether ketone sulfone)s organic matrix (C-SPAEKS) were synthesized. Modified GO nanosheets (ATP@GO) was synthesized by using GO as a template, then chemically bonded adenosine triphosphate (ATP) on GO nanosheets. Modified ATP@GO and composite membranes were characterized by FT-IR, 1 H NMR, SEM and XPS. These composite membranes exhibit outstanding proton conductivity, thermal stability and dimensional stability. Compared to C-SPAEKS membranes (32.3 mS cm −1 at 20 °C, 108.9 mS cm −1 at 90 °C), C-SPAEKS/ATP@GO-1 membrane showed enhanced proton conductivity (50.0 mS cm −1 at 20 °C, 184.8 mS cm −1 at 90 °C). Meanwhile, the open circuit voltage (OCV) and power density of C-SPAEKS/ATP@GO-1 were 0.9941 V and 466.33 mW/cm 2 , respectively, which were much higher than the C-SPAEKS (0.8973 V, 190.72 mW/cm 2 ), showing good fuel cell performance. The results show that functionalized GO could make an important contribution to proton conduction and improvement of comprehensive performance in composite membrane, which indicate that these composite membranes have the potential to be used as PEMs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Xiaowei Liu,Peng Chen,Xiangdong Li,Jiaen Zhong,Kexin Li,Miaomiao Ye,Lili Wang
The widespread implementation of ultrafiltration (UF) technology, which has gained popularity for drinking water treatment, has been impeded by rising operational costs and shortened membrane lifespans resulting from membrane fouling. Here, an integrated pretreatment technique combining oxidation, adsorption, and coagulation was developed using the S(IV)–Fe(II) binary activated permanganate (PM) system, S(IV)–Fe(II)/PM. The efficacy of S(IV)–Fe(II)/PM pretreatment in mitigating UF membrane fouling was investigated for various raw water sources, including lakes, rivers, and seawater. The operational parameters of S(IV)–Fe(II)/PM pretreatment were optimized, and the underlying mechanisms for fouling alleviation were explored. Relative to conventional pretreatment methods, S(IV)–Fe(II)/PM pretreatment reduced reversible fouling-induced resistance by 13%–92% and irreversible fouling-induced resistance by 11%–86%. The S(IV)–Fe(II)/PM system exhibited optimal mitigation of membrane fouling at a PM:S(IV):Fe(II) dosage ratio of 2:3:3, with G rapid × T rapid = 45948, G slow × T slow = 12480, and a settling time of 30 min (where G is the velocity gradient and T is contact time). The effectiveness of S(IV)–Fe(II)/PM pretreatment in controlling UF membrane fouling can be attributed to the following mechanisms: 1) modification of feed water quality in terms of organic compound characteristics and concentration, colloidal particle quantity and size distribution, and microbial activity and quantity; and 2) adjustment of the membrane surface deposition environment, resulting in reduced polysaccharide and protein content, particle size distribution range, and biomass, as well as alterations in physicochemical properties such as hydrophilicity and interfacial free energy. This study highlights the efficacy of S(IV)–Fe(II)/PM pretreatment in ensuring high-quality UF effluent while effectively reducing membrane fouling, especially its potential for alleviating irreversible membrane fouling.
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POLYMER BULLETIN
·
2023
·
IF 3.2
Chen Zhengpeng,Li Jie,Guo Hongyun,Zhang Yongdong,Ma Mingzhong,Zhou Xing,Yao Wenhuan,Ma Hengchang,Lei Ziqiang,Lu Dedai
Transcatheter arterial embolization has been used clinically for the treatment of intermediate to advanced unresectable tumors, which is a complex procedure and may pose other risks. In order to achieve an efficient and simple therapeutic diagnostic method for tumors, this paper is based on the fact that the fluorescence properties of AIE fluorescent molecules are similar to those of pH-responsive polyamino acid materials undergoing a “sol–gel” phase transition in a tumor micro-acid environment, and two polyamino acid materials, PGTTC and PGCLTGCL, were linked with TPA derivatives of AIE fluorescent molecules to obtain catheter-free embolic agents, PGTTC-DCDPP-2TPA and PGCLTGCL-DCDPP-2TPA. In tumor fluorescence imaging experiments in tumor-bearing mice, both were enriched at the tumor 72 h after injection and that of the PGCLTGCL-DCDPP-2TPA was stronger, moreover, the tumor cells were suppressed and necrotic after 25 days. Therefore, this pH-responsive noninterventional embolization combination therapeutic diagnostic system has good prospects for application in the field of combined therapeutic diagnostic multifunctional platforms.
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ENERGY & FUELS
·
2023
·
IF 5.3
Lishi Bao,Chenguang Bao,Qifeng Sun,Jiaxin Zou,Hongbo Liu,HuiChen
Transition metal-doped carbon catalysts are expected to replace noble metal catalysts for the oxygen reduction reaction (ORR). In this paper, a ZIF layer consisting of Co and Cu was formed on the surface of silica nanospheres, and then heteroatom S was added to obtain a porous carbon material catalyst (Co/Cu-NSC) after pyrolysis. Due to its porous structure, the Co/Cu-NSC catalyst has a large number of active sites with excellent ORR catalytic performance. The limiting current density of the Co/Cu-NSC catalyst is as high as 6.25 mA cm–2 (5.91 mA cm–2 of commercial Pt/C catalyst). The half-wave potential and onset potential of the Co/Cu-NSC catalyst are comparable to those of commercial Pt/C catalyst, and it has better stability and methanol resistance than commercial Pt/C catalyst. In addition, the Co/Cu-NSC catalyst affords excellent performance in a zinc–air battery, achieving high power density (145 mW cm–2) and continuous charge–discharge time (177 h) at 5 mA cm–2.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Huijie Wang,Qi Liu,Mengyang Xu,Chenlong Yan,Xianghai Song,Xin Liu,Huiqin Wang,Weiqiang Zhou,Pengwei Huo
The localized surface plasmon resonance (LSPR) effect has shown significant progress in enhancing the efficiency of light absorption and separating photogenerated carriers. Herein, the dual-plasma enhanced 2D/2D/2D g-C 3 N 4 /Pd/MoO 3-x (CPM) S-scheme heterojunction photocatalysts were synthesized using the method of hydrothermal and electrostatic self-assembly for high-selectivity photocatalytic reduction of CO 2 to produce CO. The dual LSPR effect of MoO 3-x and ultrathin Pd nanosheets synergistically broadened the optical response range of the CPM composites and successfully improved the photocatalytic activity and near-infrared (NIR) performance. The optimized CPM-30 photocatalysts exhibited CO yields of 18.55 μmol g −1 with a selectivity of 96.3%. In addition, the CO yield reached 3.92 μmol g −1 after 4 h of NIR light photoirradiation. The electron spin resonance (ESR) and ultraviolet photoelectron spectroscopy (UPS) tests showed that the S-scheme heterojunctions were constructed by coupling g-C 3 N 4 /Pd nanosheets and MoO 3-x . This work will provide a reference for improving product selectivity through the design of two-dimensional composites and the utilization of plasma materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Xuanning Qin,Han pang,Zebin Yu,Zuoyu Qin,Ronghua Jiang,Shuangquan Yao,Jun Huang,Yanping Hou,Ben Fan
Accelerating electron transfer and exposing active sites are key factors that could improve electrocatalytic hydrogen evolution reaction (HER). In this study, Co 3 S 4 -Ni 3 S 2 -C/N, the cactus bulb-shaped nanoparticles based on metal-organic frameworks (MOFs), were successfully prepared. The catalyst requires only 101 and 227 mV overpotential to reach current densities of 20 and 100 mA cm −2 , respectively, in 1 M KOH. The high catalytic activity is attributed to the confinement effect achieved by introducing 2-aminoterephthalic acid as a precursor, allowing the catalyst to have a small particle size and fully exposed metal active sites. Moreover, the catalyst has a highly conductive metal-S-C/N channel that effectively reduces the intrinsic charge transfer resistance of the catalytic electrode, improves its conductivity, and modulates the electron density at the metal active site. Furthermore, compared to other crystal planes, the exposed (111) crystal plane of Co 3 S 4 provides the most octahedral coordination of high spin state Co 3+ , which is highly catalytically active. This makes it the dominant crystal plane for catalysis. Through spatial confinement effect to limit metal sulfide particle size and introducing an organic backbone to create highly conductive metal-S-C/N channels, our study provides a general approach to developing highly active catalytic materials.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Shengwang Chen,Xiaoli Sheng,Yanyun Wang,Pingping Yu,Chenghan Yang,Xian Zhang,Hao Fang,Yiwei Zhang,Yuming Zhou
Nitrogen-rich C 3 N 5 has emerged as a promising visible light catalyst due to its narrow band gap. Nevertheless, its practical application is hindered by the rapid recombination of photogenerated carriers. To address this limitation and enhance the photocatalytic performance of C 3 N 5 -based photocatalysts, one effective measure involves the construction of heterojunctions in conjunction with other semiconductors. In this work, the C 3 N 5 /TiO 2 S-scheme photocatalysts was constructed by matching C 3 N 5 with a more negative conduction band (CB) and TiO 2 with a more positive valence band (VB). Photoelectric tests exhibited that the prepared photocatalysts possessed enhanced visible light photoresponsivity as well as excellent charge separation and transport efficiencies. The characterization results of XPS and EPR confirmed that the existence of internal electric field and the unique S-scheme charge transfer mechanism, which achieves overall spatial separation of effective photogenerated carriers and accelerates the recombination of redundant electrons and holes. The photocatalytic hydrogen production performance of the TCN2 is 6.9 times and 30 times higher than that of C 3 N 5 and TiO 2 , respectively, which is ascribed to the unique charge transfer mechanism of the S-scheme heterojunction and significantly enhanced photocatalytic activity. The simple construction of S-scheme heterojunctions in this work provides a new strategy for research in other fields.
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Small
·
2023
·Vol. 20
·期 7
·2306820
·
IF 13.3
Zheng Zheng,Bing Wang,Zhuo Li,Hong Hao,ChaoYang Wei,WenYu Luo,LinYu Jiao,Sheng Zhang,Bo Zhou,XiaoXun Ma
Constructing heterojunction of supramolecular arrays self-assembled on metal–organic frameworks (MOFs) with elaborate charge transfer mechanisms is a promising strategy for the photocatalytic oxidation of organic pollutants. Herein, H 12 SubPcB–Br (SubPc–Br) and UiO-66 are used to obtain the step-scheme (S-scheme) heterojunction SubPc–Br/UiO-66 for the first time, which is then applied in the photocatalytic oxidation of minocycline. Atomic-level B–O–Zr charge-transfer channels and van der Waals force connections synergistically accelerated the charge transfer at the interface of the SubPc–Br/UiO-66 heterojunction, while the establishment of the B–O–Zr bonds also led to the directional transfer of charge from SubPc–Br to UiO-66. The synergy is the key to improving the photocatalytic activity and stability of SubPc–Br/UiO-66, which is also verified by various characterization methods and theoretical calculations. The minocycline degradation efficiency of supramolecular SubPc–Br/UiO-66 arrays reach 90.9% within 30 min under visible light irradiation. The molecular dynamics simulations indicate that B–O–Zr bonds and van der Waals force contribute significantly to the stability of the SubPc–Br/UiO-66 heterojunction. This work reveals an approach for the rational design of semiconducting MOF-based heterojunctions with improved properties.
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