APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xianbo Yu,Feng Yan,Yang Zhao,Bo Geng,Xinzhi Ma,Lili Wu,Xitian Zhang,Yujin Chen
The inferior hydrogen evolution reaction (HER) catalytic performance of MoS 2 can be attributed to its small edge ratio, large inert substrate surface, and poor electrical conductivity, while the multiple strategies are expected to be employed simultaneously to modulate the electronic structure of MoS 2 and yield catalysts with superior HER catalytic performance. Here, we report a MoS 2 containing a 1 T phase with expanded layer spacing and construct it as a heterostructured material with MoO 2 (MoO 2 @E-MoS 2 ). Specifically, the presence of the 1 T phase and expanded layer structure of MoS 2 can enhance electrode conductivity, increase active site exposure, promote H 2 O adsorption, and optimize the Gibbs-free energy of hydrogen. The constructed heterostructure can modulate the electronic structure of the catalyst, enhance electron transfer at the interface, elevate water adsorption energy, and reduce the hydrogen reaction energy barrier. Moreover, density functional theory calculations indicate that the S site of MoS 2 in this catalyst exhibits a higher affinity for H 2 O adsorption, while the Mo site demonstrates a greater capacity for H* adsorption/desorption. Ultimately, MoO 2 @E-MoS 2 shows low overpotentials of 93 and 99 mV at a current density of 10 mA cm −2 , as well as exceptional long-term stabilities exceeding 70 and 130 h at current densities ranging from 10 to 30 mA cm −2 in acidic and alkaline media, respectively.
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高影响因子
Catalysts
·
2023
·Vol. 13
·期 11
·1426
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IF 3.9
Shihu Zhu,Tiantian Liu,Shuang Yu,Huijing Yang,Qimeng Sun,Jin You Zheng
The hydrothermal method is a frequently used approach for synthesizing HER electrocatalysts. However, a weak tolerance to high temperature is an intrinsic property of carbon cloth (CC) in most situations, and CC-based catalysts, which require complex technological processes in low-temperature environments, exhibit weak stability and electrochemical performance. Hence, we provide a new solution for these issues. In this work, MoO3-NiSxfilms of 9H5E-CC catalysts are synthesized, first through electrodeposition to form Ni particles on CC and then through a hydrothermal reaction to reform the reaction. The advantages of this synthetic process include mild reaction conditions and convenient operation. The obtained MoO3-NiSxfilm presents excellent catalytic activity and stability for HER. MoO3-NiSxfilm requires only a low overpotential of 142 mV to drive 10 mA cm−2for HER in 1.0 m KOH, and the obtained 9H5E-CF film only needs 294 mV to achieve 50 mA cm−2for OER. Remarkably, they also show excellent OER, HER, and full water splitting long-term electrochemical stability, maintaining their performance for at least 72 h. This work can be expanded to provide a new strategy for the fabrication of stable, high-performing electrodes using simple, mild reaction conditions.Keywords:hydrothermal reaction;MoO3-NiSxfilm;electrodeposition and reforming reaction;anodizing
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NEW JOURNAL OF CHEMISTRY
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2023
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IF 3.3
Jianzhao Cao,Rui Li,Ying Qi,Zhaoxiang Qi,Junzi Huang,Yahong Xie
Perovskite oxides are considered promising efficient and cost-effective water splitting electrocatalysts under alkaline conditions because of their excellent hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activity. However, due to their poor electron transfer and lack of exposed active sites, their HER activity is still much lower than that of precious metal catalysts. Besides, to date, few studies have been reported on the HER in complex water systems. In this study, a new composite electrocatalyst, SrCo0.7Fe0.3O3−δ@CdS, with a core–shell structure (denoted as SCF@CdS) was successfully prepared using an in situ coprecipitation method, which exhibited efficient HER activity in an alkaline environment and oilfield wastewater. The better electrocatalytic performance of SCF@CdS than pure SCF can be attributed to the larger specific surface area and more exposed active sites in this core–shell structure, and the lone pair electrons from S in CdS can also form coordination bonds with the vacant orbital of Co in the perovskite by sharing electron pairs, thus increasing the concentration of oxygen vacancies. This study provides a strategy to improve the HER performance of perovskite catalysts in complex water systems via the construction of a core–shell structure.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
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IF 9.8
Linfeng Peng,Hui Li,Wangjun Lin,Tangfu Xiao,Jianqiao Wang,Jinfeng Tang,Nana Wang
Antimony (Sb) pollution in water has attracted extensive attention due to the biotoxicity of Sb. Secondary iron minerals readily sorb heavy metal(loid)s and critically affect their cycling in terrestrial environments. However, compared with synthetic pure iron mineral phases, little is known about the Sb sorption behavior and mechanism on natural secondary iron minerals (nSIMs) composed of various mineral phases. In this study, sorption experiments were conducted to investigate the Sb(V) sorption properties of nSIMs from an acid mine drainage zone and corresponding single-component synthetic secondary mineral phases and to compare their sorption behaviors and mechanisms. Spectroscopic analyses indicated that the nSIMs structurally resembled a hybrid of schwertmannite , jarosite and goethite . Sb(V) sorption on nSIMs, schwertmannite, goethite and jarosite was controlled by chemisorption , with maximum Sb(V) sorption capacities of 217.39, 233.65, 32.17 and 35.61 mg/g, respectively. nSIMs demonstrated an excellent Sb(V) sorption capacity equivalent to or greater than that of the single-component phases. XRD, FTIR and Raman analyses indicated that Sb(V) was immobilized on nSIMs mainly through ion exchange with structural SO 4 2− and complexation interactions with surface Fe O and Fe OH; then, an Fe O Sb surface phase formed during the dissolution and further transformation of schwertmannite and jarosite into goethite. SEM revealed that nSIMs had an advantage in surface microstructure over the single components. These results suggested that despite the similarities in Sb(V) binding mechanism between nSIMs and schwertmannite, nSIMs might be more reactive for Sb(V) sorption since the nSIM components could mutually influence each other and facilitate Sb(V) sorption. This research suggests that nSIMs have potential for Sb(V) removal and helps elucidate the environmental behavior of Sb(V) associated with nSIMs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Yinghong Ji,Xiaoyan Ding,Yanjun Xue,Jingjing Wang,Jian Tian
The formation of composites by loading co-catalysts on semiconductor photocatalysts to improve hydrogen (H 2 ) evolution performance is a feasible strategy. Metallic 1T phase molybdenum disulfide (MoS 2 ) as cocatalysts were decorated on zinc indium sulfide (ZnIn 2 S 4 ) nanoflowers by a grinding method to construct 1T-MoS 2 @ZnIn 2 S 4 composites. The H 2 production rate of 1T-MoS 2 @ZnIn 2 S 4 composites with optimum 7 wt% 1T-MoS 2 loading achieves 15.6 mmol g −1 h −1 , 5.5 times higher than ZnIn 2 S 4 nanoflowers. The apparent quantum efficiency (AQY) increases from 3.1 % (ZnIn 2 S 4 nanoflowers) to 13.0 % (1T-MoS 2 @ZnIn 2 S 4 composites) under the wavelength light irradiation at λ = 370 nm. The loading of metallic 1T-MoS 2 with abundant edge and substrate active sites on ZnIn 2 S 4 can enhance visible light absorption, promote the transfer of electrons, and inhibit carrier recombination, thereby improving photocatalytic performance. This work offers inspiration for the design of composite photocatalysts with efficient photocatalytic capabilities.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2023
·
IF 9.8
Xiaodan Zhao,Jiahui Wei,Ying Wu,Zuoming Zhou,Guohua Jing
Sulfite autoxidation in combination with the cobalt-based heterogeneous activators, has recently emerged as the efficient sulfate radical (SO 4 •− ) generation process for organic micropollutant abatement in the water and wastewater treatment , yet the sluggish >Co(II)/Co(III) redox cycling currently compromises the efficacy of radical generation and the potential applications. Herein, regarding that the reductive W(IV) species in WS 2 can modulate the >Co(II)/Co(III) redox cycling in the advanced oxidation processes , confinement of cobalt with WS 2 (Co-WS 2 ) is designed and characterized. The Co-WS 2 /sulfite process achieves an ultrafast tetracycline (TC) abatement (∼100 % abatement of TC within 1 min) under circumneutral conditions with lower dosage of sulfite and activator, outperforming the current cobalt-based heterogeneous counterparts. The dominant reactive radicals are identified as SO 4 •− and hydroxyl radical (HO • ), which are quantified to be 9.7 μM and 4.5 μM, respectively. The superior radical generation efficiency and the concomitant TC abatement rely on the excellent redox properties and electron transfer capability of Co-WS 2 . The inter-transformation of >Co(II)/>Co(III) can be accelerated via the involvement of the reductive W(IV) species with the redox-reversibility of the W(IV)/W(VI) couple in the presence of sulfite. The TC degradation intermediates and the corresponding pathways are also proposed according to the ultra-performance liquid chromatography and quadrupole-time of flight mass spectrometry (UPLC-QTOF-MS) analysis. In addition, the influences of the reactant dosage, coexisting anions (HCO 3 − , HPO 4 2− , Cl − and NO 3 − ), humic acid and the various real water matrices on TC abatement are thoroughly explored. Especially, the Co-WS 2 /sulfite process is advantageous owing to the negligible effect of the coexisting anions on the TC abatement. This study provides a novel heterogeneous activator for significantly improving sulfite activation efficacy to achieve the efficient organic micropollutant abatement.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Changcheng Cui,Junjie Fu,Dongxing Kou,Yimeng Li,Hao Wei,Zucheng Wu,Wenhui Zhou,Zhengji Zhou,Shengjie Yuan,Yafang Qi,Shuping Pang,Zhipeng Shao,Sixin Wu,Guanglei Cui
The Cu 2 ZnSn(S,Se) 4 solar cells (CZTSSe) are emerging as a hot area of low-cost thin film photovoltaic technology owing to its non-toxicity and excellent photoelectric properties. However, the large open-circuit voltage deficit ( V oc,deficit ) caused by the inherently defective CdS/ CZTSSe heterojunction interface is still a huge challenge for improving power conversion efficiency. Herein, we reconstruct the heterojunction interface by inserting a CZTSSe:In into the CdS/CZTSSe heterojunction through an In 2 Se 3 post-deposition treatment. The local occupation of In 3+ at Zn 2+ and Sn 4+ sites decreases the disordered Zn- and Sn-related deep defects and generates benign In Zn donors within CZITSSe transition layer simultaneously, which effectively enhances the surface p-to-n conversion. The combination of chemical and field-effect passivation regulates the charge extraction and passivates the charge recombination. As a result, the In element-buried absorber enables the V oc boost from 488 to 527 mV with an impressive active-area efficiency of 13.59 %. These results demonstrate the great potential of the In element-buried absorber in alleviating the V oc,deficit and enhancing the performance of CZTSSe solar cells.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Wenwen Bie,Shuzhao Zhang,Lin Zhang,Hengye Li,Xiaoyu Sun,Tianpei Cai,Zhongxia Wang,Fenying Kong,Wei Wang
Herein, a thioether-functionalized porous β-cyclodextrin polymer (P(Bn-S-CD)) was prepared for efficient removal of heavy metal ions and organic micropollutants (OMPs) from water. P(Bn-S-CD) showed a surface area of 763 m 2 /g and a sulfur content 5.83 wt%. Based on screening studies, Hg 2+ and diclofenac sodium (DS) were selected as model pollutants. P(Bn-S-CD) could adsorb Hg 2+ and DS simultaneously, while the adsorbed Hg 2+ afforded positive charges to the primary rims of CDs, greatly enhancing the adsorption rate and adsorption capacity of DS. Although the adsorbed DS showed no obvious effect on Hg 2+ adsorption, it improved the affinity of Hg 2+ upon P(Bn-S-CD). Adsorption mechanism studies confirmed the essential role of electrostatic interactions for these results. P(Bn-S-CD) also showed good selectivity towards heavy metal ions, excellent adsorption performance in real water at environmental levels and good reusability, implying great promise for water treatment.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2023
·Vol. 34
·期 32
·1-11
·
IF 2.8
Hou Shikun,Wang Ying,Gao Feng,Jin Fei,Liang Weijie,Ge Zhizhou,Bai Gongxun,Peng Xiao,Yang Hua
Carbon cloth-based electromagnetic wave (EMW) absorbing materials have been widely studied due to their advantages of light weight, flexibility and high strength. At present, researchers widely use chemical in-situ growth method to construct secondary components on the surface of fibers to adjust the EMW absorption properties of carbon cloth (CC). However, there is still a lack of theoretical support behind this behavior. Herein, SnO 2 @SnS 2 was used as the secondary component, and SnO 2 @SnS 2 was constructed on the surface of CC by physical mixing (PM) and chemical in-situ (IS) growth, and the influence of the interface construction method on the microwave absorption performance of CC composites was studied. It is found that compared with SnO 2 @SnS 2 /CC-PM, SnO 2 @SnS 2 /CC-IS can more effectively adjust electromagnetic parameters, enhance multiple polarization, and enhance EMW loss. This can be attributed to the fact that the heterointerface between the secondary component constructed by chemical in-situ growth and the CC (SnO 2 @SnS 2 /CC) contributes much more to the EMW absorption than the intrinsic heterostructure in the secondary component (SnO 2 /SnS 2 ). It is proved that chemical in-situ growth is a more effective strategy to construct high-performance EMW absorbing materials. Provide research theoretical support for the development of high-performance CC composites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Hengcong Tao,Tianbo Jia,Lina Zhang,Xin Li,Panfeng Li,Yingtang Zhou,Chunyang Zhai
Electrochemical carbon dioxide reduction (ECR) is a commercially promising technology to resolve the energy dilemma and accomplish carbon recycling. Herein, a novel electrocatalyst has been investigated to produce formate (HCOOH) highly selectively during ECR by loading SnO 2 @C onto cuprous sulphide (Cu 2 S) to form a triplet effect at the interface. Snowflake-like Cu 2 S significantly enhances the local concentration of carbon dioxide (CO 2 ) and promotes the binding of CO 2 with SnO 2 , and the addition of carbon spheres enhances the electron transport, which is beneficial to the conversion of CO 2 to HCOOH products. The snowflake-like Cu 2 S loaded with 1 wt% SnO 2 @C had an HCOOH Faraday Efficiency of 88% at −1.0 V ( vs. Reversible Hydrogen Electrode, RHE), and the current density for CO 2 reduction was stabilized at 15.6 mA cm −2 , which was much higher than the HCOOH Faraday efficiency (FE) of 31.0% for pure Cu 2 S accompanied by a CO 2 reduction current density of 3.9 mA cm −2 . Combined investigations using in-situ Fourier transform infrared spectroscopy (FT-IR) with in-situ Raman spectra reveal that the active species is Cu + . Cu 2 S/1%SnO 2 @C can effectively promote the adsorption and activation of carbonate and inhibit the production of CO intermediates. The corresponding density functional theory (DFT) demonstrates that Cu 2 S/1%SnO 2 @C can well stabilize the HCOO* intermediate during the ECR process. The interaction between Cu 2 S and SnO 2 @C adjusts the surface electronic distribution and accelerates electron transfer, which efficiently improves CO 2 -to-HCOOH conversion. The result obtained from this work provides a simple and efficient electrocatalyst to enhance the HCOOH selectivity of ECR.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Mengwei Guo,Bo Zhang,Qibo Zhang
In this work, sulfur-doped manganese (S-Mn/CP) pre-catalysts supported by carbon paper (CP) were prepared from choline chloride/ethylene glycol-based deep eutectic solvent containing different manganese salts via electrodeposition method. The effect of anions, including NO 3 – , Cl - , SO 4 2- , CH 3 COO – , and crystal water (H 2 O), on the evolution of the structure and OER activity of as-prepared Mn-based pre-catalysts was analyzed. It turns out that the NO 3 – and H 2 O can be reduced during the electroreduction of Mn(II) species and induce the formation of manganese oxide/hydroxide. Thiourea (TU), used as a sulfur source, decomposes at the cathode and releases S 2- . The TU and H 2 O replace the Cl - in the [Mn(Cl) 6 ] 4- to form [Mn(Cl) 6- x (H 2 O) x ] x -4 and [Mn(Cl) 6- x - y (TU) y (H 2 O) x ] x + y -4 complexes, promoting the electroreduction of Mn(II) species. The OER intrinsic catalytic activity of the amorphous Mn 3 O 4 pre-catalyst is 16.3 times lower than that of the metallic Mn 0 pre-catalyst in a 1.0 M KOH solution. After annealing in an argon atmosphere, the surface of metallic Mn 0 is in-situ converted into Mn 3 O 4 and exhibits superior activity (0.0395 A g −1 cm -2 ECSA ) than the ordinary Mn 3 O 4 electrode (0.0088 A g −1 cm -2 ECSA ). This study brings insights into the effect of anion on the evolution of structure-activity of Mn-based pre-catalysts during the electrodeposition and OER catalytic process.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Zheng Liu,Hong Ding,Lin Qi,Jing Wang,Yubao Li,Limin Liu,Ganjun Feng,Li Zhang
Developing bone implants with dynamic self-adjustment of antibacterial, angiogenic, and osteogenic functions in line with a bone regenerative cascade is highly required in orthopedics. Herein, a unique core–shell nanorods array featuring a thin layer of NiS coated on each SrTiO3 nanorod (NiS@SrTiO3) was in situ constructed on titanium (Ti) through a two-step hydrothermal treatment. Under near-infrared (NIR) irradiation, the photoresponsive effect of NiS layer in synergy with the physical perforation of SrTiO3 nanorods initially enabled in vitro antibacterial rates of 96.5% to Escherichia coli and 93.1% to Staphylococcus aureus. With the degradation of the NiS layer, trace amounts of Ni ions were released, which accelerated angiogenesis by upregulating the expression of vascular regeneration-related factors, while the gradual exposure of SrTiO3 nanorods could simultaneously enhance the surface hydrophilicity in favor of cell adhesion and slowly release Sr ions to promote the proliferation and differentiation of MC3T3-E1 cells. The in vivo assessment verified not only the satisfactory antibacterial effect but also the superior osteogenic ability of the NiS@SrTiO3/Ti group with the aid of NIR irradiation, finally promoting the osseointegration of the Ti implant. The modification method endowing Ti implant with antibacterial, angiogenic, and osteogenic functions provides a new strategy to improve the long-term reliability of Ti-based devices.
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