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ACTA MATERIALIA · 2023 · IF 9.4

An all-lithium-metal-oxides-based low temperature solid oxide fuel cell with triple (H+/O2−/Li+) conducting electrolyte

Ruineng Ruan,Haibo Xiao,Wenjing Dong,Zhanghong Yu,Xunying Wang,Baoyuan Wang,Chen Xia,Hao Wang

Fast ionic transportation is in high demand for developing low-temperature solid oxide fuel cells (LT-SOFCs). Facing this challenge, a new H + /O 2− /Li + triple conductor is designed in this study from a lithium-metal oxide, spinel Li 4 Ti 5 O 12 (LTO). First-principle calculation based on density functional theory (DFT) reveals the proton transport barrier in LTO can be as low as 0.37 eV while the barrier for oxygen ion transportation is 0.94 eV. Using the designed LTO as the electrolyte and a typical cathode of lithium-ion battery, LiNi 0.8 Co 0.15 Al 0.05 O 2-δ , as the symmetrical electrodes, an all-lithium-metal-oxides-based LT-SOFC is constructed. High performance is achieved by the SOFC at 550–425 °C, i.e. 625 mW cm −2 at 550 °C, and a low activation energy of 0.60 eV is found with respect to the ionic conductivity of LTO at 550–475 °C. Further study confirms the dual O 2− /H + conduction of LTO via the application of proton and oxygen ion filters as well as the transference number test. Additionally, particular attentions are paid to the transport behavior of Li + in the cell via a charging process study and from XRD results. The possible contribution of triple conduction on fuel cell performance is discussed. This work demonstrates the great promise of triple H + /O 2− /Li + conducting lithium-metal oxides for LT-SOFC electrolyte development.

CAS / MDL: 13463-67-7
研究领域: 材料科学 · 能源技术
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ACS Catalysis · 2025 · IF 13.1

Ag–Co Dual Sites-Decorated TiO2 Enabling Accelerated Electron Transfer for Selective Photocatalytic Oxidative Coupling of Methane

Weina Yang,Yachao Wang,Yaxiong Wei,Guofeng Zhao,Weixin Huang,Cong Fu

Photocatalytic oxidative coupling of methane (OCM) offers a sustainable pathway for direct conversion of methane into value-added hydrocarbons, yet faces persistent challenges in balancing efficient methane activation with suppression of overoxidation. Here, we present a TiO2-based photocatalyst decorated with highly dispersed Ag–Co dual sites that achieves superior performance in continuous-flow OCM. The optimized AgCo–TiO2 system demonstrates a remarkable C2 hydrocarbon production rate of 1.7 mmol g–1 h–1 with 91% selectivity while maintaining stable operation for over 30 h. In situ spectroscopic analyses indicate that the introduced Co species induce mobile-charge imbalances, driving the directional transfer of photogenerated electrons and effectively suppressing electron–hole recombination. Coupled with Ag serving as a catalytic center, these effects synergistically enhance O2 activation, C–H bond cleavage, and selective C–C coupling, thereby contributing to the superior catalytic performance. This work provides valuable mechanistic insights into the photocatalytic OCM process, highlighting the pivotal role of precisely engineered charge transfer pathways in enabling efficient methane-to-C2 conversion.

CAS / MDL: 13463-67-7
研究领域: 光催化 · 材料科学 · 化学工程 · 环境化学 · 能量转换
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JOURNAL OF POWER SOURCES · 2019 · IF 7.467

Boosting electrocatalysis by heteroatom doping and oxygen vacancies in hierarchical Ni-Co based nitride phosphide hybrid

Zhiyu Shao,Jing Sun,Niankun Guo,Feng He,Keke Huang,Fuli Tian,Qin Wang

Designing highly active and low-cost electrocatalysts towards oxygen evolution reaction has ignited much interest in recent years. Thereby, rational design of those catalysts is an urgent topic that must be addressed. Herein, an effective strategy is demonstrated to be beneficial to the formation of hierarchical nitride phosphide hybrid with abundant oxygen vacancies . This hybrid catalyst exhibits an excellent OER catalytic performance, as demonstrated by an ultralow Tafel slope of 41 mV·dec −1 and an overpotential of 290 mV at 10 mA cm −2 in 1.0 M KOH solution, which is superior to those of the pure nitride, phosphide, and the commercial IrO 2 catalysts. The outstanding catalytic performance can be attributed to the specific heterojunction structure, accessible active sites, and abundant oxygen vacancies, which can facilitate the charge transport and the release of the O 2 bubbles. This study not only provides a facile strategy for constructing surface oxygen vacancies onto phosphide/nitride hybrid, but also exhibits an insight into the nature of hierarchical electrocatalyst with multiple active sites.

研究领域: 电化学 · 材料科学 · 催化
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Disorder–order structure of a-CeO2/SnFe2O4 heterojunction with enhanced exciton dissociation for the NIR-driven photocatalysis

Hao Jiang,Mei Yan,Hao Chen,Yutuo Fu,Chongshen Guo

Strong Coulomb force between photogenerated electrons and holes often results in high level exciton pairs during the photocatalytic process, which hinders the formation of reactive oxygen species (ROS) in the photocatalytic reaction, particularly for the photocatalysis under near infrared (NIR) irradiation. Hence, it is crucial to dissociate excitons into free carriers. In this study, we propose a novel amorphous–crystalline heterojunction of a-CeO 2 /SnFe 2 O 4 for the NIR-driven photocatalytic degradation and sterilization. The introduction of disorder–order interface in heterojunction could greatly enhance the built-in electric field, thereby serving for exciton dissociation. Additionally, the presence of oxygen vacant sites in the a-CeO 2 /SnFe 2 O 4 system can effectively modulate the electronic structure of the material, facilitating exciton dissociation in conjunction with the built-in electric field. The DFT simulation proved the positive impact of the disorder–order interface on charge separation, as well as its enhancement on the activation of O 2 and H 2 O molecules. This work provides a theoretical support for the creation of disorder–order interface to promote exciton dissociation and enhance photocatalytic performance.

CAS / MDL: 10294-41-4 10025-69-1
研究领域: 材料科学 · 光催化 · 表面化学 · 理论化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Anthraquinone centers modified covalent organic frameworks for boosted photocatalytic O2-to-H2O2 synthesis: Inhibiting the in-situ decomposition of H2O2

Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han

Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.

研究领域: 材料科学 · 环境科学 · 化学工程
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CATALYSIS TODAY · 2024 · IF 5.2

The high-entropy oxide-promoted oxidative condensation reaction of biomass-derived furfural with aliphatic alcohol in the presence of O2

Jipeng Wang,Xinli Tong,Chen Guo,Yahui Wei

The high entropy oxides are widely studied as the potential catalytic materials owing to their unique structure and excellent properties. In this work, a new high entropy oxide catalyst MnFeCoNiCuO x was successfully prepared and used for the oxidative condensation reaction of furfural (FUR) and aliphatic alcohol , where the carbon-chain length can be selectively increased under the mild conditions. For the selective oxidative transformation of FUR with n-butanol, a more than 99.0 % conversion of FUR and 91.5 % selectivity of 2-(furanyl-2-methylene) butanal was obtained at 80 ºC for 2 h. In addition, the oxidative condensation of FUR with ethanol, n-propanol, n-pentanol, n-hexanol and n-heptanol was also carried out with the MnFeCoNiCuO x - LiOH as catalyst system in the presence of molecular oxygen , where a moderate to high product yields were acquired. Furthermore, the characterizations of catalyst showed that the existence of abundant oxygen vacancy and high specific area was greatly important to the catalytic reactions .

研究领域: 化学工程 · 催化科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

Synthesis and performances of biomass carbon@Li(Ni0.6Co0.4)O2 micron-tube as electrode material in aqueous lithium-ion hybrid supercapacitors

Yajuan Jiang,Shining Zhang,Chunyu Xu,Bin Jia,Shijie Ren,Wenyu Zheng,Yicong Huang,Kunpeng Jiang,Xiuyun Zhang,Yunyun Zhao,Guisheng Zhu,Huarui Xu

In this paper, biomass carbon@Li(Ni 0.6 Co 0.4 )O 2 (BC@LNCO) micron-tube is successfully synthesized via a bio-templating method as cathodic material for lithium-ion hybrid supercapacitors. Cobalt nickel subcarbonates nanowires arrays are homogeneously grown on bagasse substrate via a unique synthesis strategy using a toluene-water interface reaction process, which subsequently transform as BC@LNCO micron-tube after lithiation process. The distinctive biomass fibre structure of bagasse biomass carbon leads to a significant enhancement in active sites in the BC@LNCO composite, which facilitates lithium-ion diffusion and enhances the contact area between the electrode and electrolyte. So, the prepared BC@LNCO electrode demonstrates improved electrical performances with a high specific capacitance of 921 F g −1 at 1 A g −1 and a good rate performance with 72 % retention at 10 A g −1 . In addition, the lithium-ion hybrid supercapacitor is fabricated with BC@LNCO and activated carbon (AC) as positive and negative electrodes, respectively. The BC@LNCO//AC device demonstrates a good energy density of 56.25 Wh kg −1 at 818.4 W kg −1 , and maintains 25.06 Wh kg −1 when the power density is up to 8143.42 W kg −1 , indicating that the prepared BC@LNCO composite can be a promising candidate as electrode material for Li-ion hybrid supercapacitor.

研究领域: 材料科学 · 能源存储
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Materials Today Energy · 2022 · IF 9.257

Suppressing the irreversible phase transition from P2 to O2 in sodium-layered cathode via integrating P2- and O3-type structures

Jingjun Zhai,Haocheng Ji,Wenhai Ji,Rui Wang,Zhongyuan Huang,Tingting Yang,Chaoqi Wang,Taolve Zhang,Ziwei Chen,Wenguang Zhao,Akhil Tayal,Lei Jin,Jun Wang,Yinguo Xiao

Layered transition metal oxides have been broadly studied due to their great potential in application as cathodes for sodium-ion batteries. However, many single-phase layered transition metal oxides, especially those crystallized in P2- or O3-type structure, possess their individual characteristics incurring unsatisfactory overall performances with respect to the reversible capacity, rate capability, and cycling stability. Here, an effective strategy of constructing the P2/O3 biphasic structure is realized in layered cathode Na 0.7 Ni 0.4 Mn 0.4 Ti 0.2 O 2 through Ti substitution. Through high-resolution scanning transmission electron microscopy and X-ray diffraction, the formation of P2/O3 intergrowth structure was clarified and the proportion of the two phases was determined. Benefitting from the presence of intergrowth structure, the layered cathode provides a competitive rate capability of 100 mAh/g at a high rate of 5 C as well as a prominent cycling stability of 80.04% capacity retention after 300 cycles at 5 C. The improved performance is closely related to the highly reversible phase transition process from P2/O3 to OP4/P3 with less strain and enhanced Na + kinetics. These findings evidence that exploring novel multiphase cathodes is an effective approach to improve the electrochemical performances of cathode for sodium-ion batteries.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Shuttle-Shape Carrier-Free Platinum-Coordinated Nanoreactors with O2 Self-Supply and ROS Augment for Enhanced Phototherapy of Hypoxic Tumor

Xu Fu,Wen Yin,Dao Shi,Yifan Yang,Suisui He,Jun Hai,Zhenqing Hou,Zhongxiong Fan,Dekui Zhang

The synergistic nanotheranostics of reactive oxygen species (ROS) augment or phototherapy has been a promising method within synergistic oncotherapy. However, it is still hindered by sophisticated design and fabrication, lack of a multimodal synergistic effect, and hypoxia-associated poor photodynamic therapy (PDT) efficacy. Herein, a kind of porous shuttle-shape platinum (IV) methylene blue (Mb) coordination polymer nanotheranostics-loaded 10-hydroxycamptothecin (CPT) is fabricated to address the abovementioned limitations. Our nanoreactors possess spatiotemporally controlled O2 self-supply, self-sufficient singlet oxygen (1O2), and outstanding photothermal effect. Once they are taken up by tumor cells, nanoreactors as a cascade catalyst can efficiently catalyze degradation of the endogenous hydrogen peroxide (H2O2) into O2 to alleviate tumor hypoxia. The production of O2 can ensure enhanced PDT. Subsequently, under both stimuli of external red light irradiation and internal lysosomal acidity, nanoreactors can achieve the on-demand release of CPT to augment in situ mitochondrial ROS and highly efficient tumor ablation via phototherapy. Moreover, under the guidance of near-infrared (NIR) fluorescent imaging, our nanoreactors exhibit strongly synergistic potency for treatment of hypoxic tumors while reducing damages against normal tissues and organs. Collectively, shuttle-shape platinum-coordinated nanoreactors with augmented ROS capacity and enhanced phototherapy efficiency can be regarded as a novel tumor theranostic agent and further promote the research of synergistic oncotherapy.

研究领域: 纳米技术 · 癌症治疗 · 生物医学工程 · 光疗 · 药学
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ACS Applied Nano Materials · 2024 · IF 5.3

Generation of •OH and •O2– Radicals by a Bi2O3-Nanoparticle/Bi4O5Br2 Type-II Heterojunction for Photocatalytic Degradation of Organic Molecules

Xiang Yu,Yuwei Mi,Zihan Gong,Yongfang Zhang,Lei Wang,Suyuan Zeng

Constructing heterojunctions is an effective strategy for increasing semiconductor photocatalytic activity. Herein, a Bi2O3/Bi4O5Br2 type-II heterojunction was synthesized using a simple one-pot solvothermal route. The 0-dimensional (0D) Bi2O3 nanoparticles are uniformly distributed within the 2D Bi4O5Br2 nanosheets with (101̅) facets dominantly exposed. In comparison with pure Bi2O3 and Bi4O5Br2, they show higher photocatalytic activity degradation of resorcinol (RO) and Rhodamine B (RhB). The Bi2O3/Bi4O5Br2 composite containing 10% Bi2O3 (BOB4) displays the best photocatalytic activity. For instance, compared with pure Bi4O5Br2 and Bi2O3, the k(RO) values of BOB4 (0.58 h–1) are 3.1 and 4.8 times higher. The enhanced photocatalytic activity is attributed to the formation of a large heterojunction interface that results from the homogeneous distribution of Bi2O3 nanoparticles in the Bi4O5Br2 nanosheet, which effectively enhances the photogenerated charge separation in a type-II mode. Major active species include superoxide radicals (•O2–), hydroxyl radicals (•OH), and holes (h+). In addition, the Bi2O3/Bi4O5Br2 photocatalysts exhibit outstanding resistance to inorganic ions, pH, water matrix, as well as outdoor sunlight and favorable stability and biocompatibility. This work presents a simple method to construct Bi-based heterojunction architectures for photoactivity improvement.

CAS / MDL: 81-88-9
研究领域: 材料科学 · 环境科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Kinetic insights into reaction pathways of acrolein formation in propylene epoxidation by H2 and O2 over Au/TS-1 catalyst

Wei Du,Zhihua Zhang,Jundi Wang,Nan Song,Xuezhi Duan,Xinggui Zhou

Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au-Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , −0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS-1 zeolite, which is absent on TS-1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro-oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.

CAS / MDL: 57-13-6 60676-86-0
研究领域: 催化化学 · 材料科学 · 环境化学
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Chemical Science · 2024 · IF 7.6

Promoting oxygen electrode reaction kinetics in photo-assisted Li–O2 batteries through heterostructure design and built-in electric field construction

Yinglei Tao,Tao Wang,Xingyu Yu,Ke Gong,Hao Gong,Haixia Chen,Xiaoli Fan,Aidi Zhang,Xianli Huang,Kun Chang,Jianping He

Li–O2 batteries (LOBs) boast an exceptionally high theoretical energy density; however, the slow kinetics of the oxygen electrode reaction have been a significant hurdle in their advancement and practical application. In this study, a composite of bismuth oxyhalide heterojunction incorporated with metal–organic frameworks (MOFs) was engineered on carbon cloth (Zr-MOF/BiOIBr/CC) as an efficient bifunctional catalyst to enhance the oxygen electrode reaction in photo-assisted LOBs. Compared to Zr-MOF/CC, Zr-MOF/BiOIBr/CC significantly expands the light absorption spectrum of the catalyst. Furthermore, the built-in electric field in the heterojunction aids in the separation and directional movement of photogenerated carriers, thereby expediting the reaction kinetics of LOBs. Consequently, the photo-assisted LOBs with Zr-MOF/BiOIBr/CC as the cathodes display a discharge potential of 3.05 V, a low charge potential of 3.20 V, and an energy efficiency of up to 95.3%, and can sustain an extended cycle life of over 255 cycles. This study underscores the potential application of MOFs/semiconductor heterostructural materials in photo-assisted LOBs and offers insights into the systematic design of photo-assisted air batteries and other advanced semiconductors.

研究领域: 材料科学 · 电化学 · 能源存储
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