Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Chen Shiyi,Zhang Shishi,Guo Lei,Pan Lun,Shi Chengxiang,Zhang Xiangwen,Huang Zhen-Feng,Yang Guidong,Zou Ji-Jun
Surface reconstruction generates real active species in electrochemical conditions; rational regulating reconstruction in a targeted manner is the key for constructing highly active catalyst. Herein, we use the high-valence Mo modulated orthorhombic Pr 3 Ir 1− x Mo x O 7 as model to activate lattice oxygen and cations, achieving directional and accelerated surface reconstruction to produce self-terminated Ir‒O bri ‒Mo (O bri represents the bridge oxygen) active species that is highly active for acidic water oxidation. The doped Mo not only contributes to accelerated surface reconstruction due to optimized Ir‒O covalency and more prone dissolution of Pr, but also affords the improved durability resulted from Mo-buffered charge compensation, thereby preventing fierce Ir dissolution and excessive lattice oxygen loss. As such, Ir‒O bri ‒Mo species could be directionally generated, in which the strong Brønsted acidity of O bri induced by remaining Mo assists with the facilitated deprotonation of oxo intermediates, following bridging-oxygen-assisted deprotonation pathway. Consequently, the optimal catalyst exhibits the best activity with an overpotential of 259 mV to reach 10 mA cm geo −2 , 50 mV lower than undoped counterpart, and shows improved stability for over 200 h. This work provides a strategy of directional surface reconstruction to constructing strong Brønsted acid sites in IrO x species, demonstrating the perspective of targeted electrocatalyst fabrication under in situ realistic reaction conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Caihong Wang,Weiliang Qi,Ying Zhou,Wandi Kuang,Tamil Azhagan,Tiju Thomas,Chunjie Jiang,Siqi Liu,Minghui Yang
Efficient semiconductor-cocatalyst junctions are of direct relevance to solar energy based fuel generation. Here, Ni-Mo ternary nitrides based one-dimensional hierarchical structures (In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni)) have been successfully prepared and used to achieve visible light driven H 2 evolution. Because of the metallic-like properties of the transition metal nitrides, Ni 0.2 Mo 0.8 N(Ni) as co-catalysts can promote photo-generated charge-carriers transportation/separation and decrease the overpotential of H 2 -evolution. Thus, the photocatalytic property of optimal 1 wt% In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni) exhibits a hydrogen evolution rate of 614.2 μmol g -1 h −1 , which is about 10 times as high as that of blank In 2 S 3 (61.4 μmol g −1 h −1 ). Besides, the pure Ni 0.2 Mo 0.8 N shows higher co-catalytic properties than Ni 0.2 Mo 0.8 N(Ni). This indicates that the metallic Ni (and related species) lowers the co-catalytic role of ternary nitrides. Another robust indication of this is the fact that In 2 S 3 -Ni 0.2 Mo 0.8 N nanohybrid displays about 2 times higher H 2 evolution rate than In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni).
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RSC Advances
·
2018
·Vol. 8
·期 49
·27686-27694
·
IF 2.936
Xue Yu,Shuying Cheng,Qiong Yan,Jinling Yu,Wen Qiu,Zhengji Zhou,Qiao Zheng,Sixin Wu
Cation substitution plays a crucial role in improving the efficiency of Cu2ZnSn(S,Se)4 (CZTSSe) solar cells. In this work, we report a significant efficiency enhancement of flexible CZTSSe solar cells on Mo foils by partial substitution of Cu+ with Ag+. It is found that the band gap (Eg) of (Cu1−xAgx)2ZnSn(S,Se)4 (CAZTSSe) thin films can be adjusted by doping with Ag with x from 0 to 6%, and the minimum Eg is achieved with x = 5%. We also found that Ag doping can obviously increase the average grain size of the CAZTSSe absorber from 0.4 to 1.1 μm. Additionally, the depletion width (Wd) at the heterojunction interface of CAZTSSe/CdS is found to be improved. As a result, the open-circuit voltage deficit (Voc,def) is gradually decreased, and the band tailing is suppressed. Benefiting from the enhanced open-circuit voltage (Voc), the power conversion efficiency (PCE) is successfully enhanced from 4.34% (x = 0) to 6.24% (x = 4%), and the Voc,def decreases from 915 to 848 mV.
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ACS Nano
·
2025
·
IF 16
Ruonan Li,Runlin Ma,Li-Li Zhang,Wei Ma,Gonglei Shao,Xu Zhang,Yun Tian,Menggai Jiao,Zhen Zhou
To tackle the challenge in electrochemical nitrogen fixing and reduction in aqueous electrolytes, the conventional approach has been to suppress the competitive hydrogen evolution reaction. Nonetheless, proton provision is a crucial step in the nitrogen reduction pathway to produce ammonia, and a single active site faces the daunting task in striking a balance between high nitrogen fixation efficiency and fast protonation kinetics. This work presents a harmonic strategy featuring atomically dispersed dual Fe–Mo sites anchored in an N-doped carbon (FeMoNC) substrate, where a low-spin Fe center with enriched empty d orbitals aids in nitrogen fixation and activation, and the adjacent Mo site accelerates the protonation kinetics of N-containing intermediates at the Fe site via a distal associative mechanism. Driven by this co-catalytic mechanism, the FeMoNC catalyst achieves a Faradaic efficiency of 37.42%, marking a significant improvement of 7.8- and 10.6-fold over Fe or Mo single-atom catalysts, respectively. Furthermore, an excellent NH3 yield of 54.40 μg h–1 mgcat.–1 is realized in a flow cell by enhancing mass transfer. This study provides valuable insights into diatomic co-catalytic mechanisms for electrochemical ammonia synthesis.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Shuo Li,Jiahe Sun,Songcheng Bo,Fangfang Yang,Kaixuan Yang,Ting Su,Hongying Lü,Zhiguo Zhu
Oxidative desulfurization (ODS) is regarded as a viable carbon–neutral way to produce sulfur-free fuels. Mo framework substituted zeolite is considered to be a potential heterogeneous catalyst to achieve this goal. Nonetheless, the hydrothermal synthesis of Mo-containing zeolite remains a challenging task in terms of theses aspects including the difficulty in isomorphous substitution of Si with Mo due to the large ionic radius of Mo (59 pm), the tendency of Mo species to precipitate in the alkaline medium, and the prolonged crystallization time. Herein, Mo-Beta zeolites were synthesized via interzeolite transformation within a short time of 24 h. The crystallization process followed the dissolution–recrystallization mechanism. Various techniques were used to confirm that Mo species was isomorphously substituted into zeolite framework. Mesopore was also created over Mo-Beta zeolite with different Mo contents. This Mo-Beta zeolites were employed as heterogeneous catalysts in oxidative desulfurization, where framework Mo species was found to be the catalytic active sites. The process parameters (catalyst dosage, reaction temperature, and H 2 O 2 amounts), reaction kinetics, and reusability were also investigated. Mo-Beta exhibited remarkably high catalyst-weight-based space–time-yield and active-site-based turnover frequency, surpassing the zeolite catalysts in the literatures. This work paves an avenue to the hydrothermal synthesis of metallosilicate zeolites for catalytic oxidations.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ruiyang Zhang,Aili Zhang,Yuehan Cao,Shuyan Wang,Fan Dong,Ying Zhou
Oxygen as an economic and ubiquitous oxidant plays a significant role in catalysis environmental remediation. However, the high thermodynamic stability of O 2 limits the practical application. Herein, we reported a novel Mo doped carbon nitride (Mo-CN/g-CN) homojunction via the in-situ growth strategy. The strong interaction between Mo-CN and g-C 3 N 4 enhanced visible-light response and photogenerated electrons and holes pairs separation, which were beneficial for photocatalytic activity. Importantly, theoretical calculation and experiments confirmed that Mo atoms on the surface of Mo-CN/g-CN could provide abundant electrons to the adsorbed O 2 to promote the generation of O 2 − , thus enhancing the photocatalytic performance. Consequently, the obtained Mo-CN/g-CN reveals excellent photocatalytic NO removal activity, demonstrating its promise for air purification. This current work gives a novel insight for O 2 activation in the application of photocatalytic environmental remediation.
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Nature Sustainability
·
2026
·
IF 32.1
Zou Xingyue,Zhang Jinzhe,Xie Jiawei,Dong Houyan,Zhou Bing,Dai Jie,Zhao Long,Wang Jiaxian,Zhan Guangming,Lian Wengao,Cao Xuelei,Liu Bingyan,Gu Xiang-Kui,Yao Yancai,Zhang Lizhi
Accelerating the global transition to sustainable green hydrogen requires highly efficient and durable industrial water electrolysis. However, the anodic oxygen evolution reaction remains a critical bottleneck. Conventional nickel-based catalysts suffer from high overpotential or rapid degradation. Here we overcome this limitation by introducing asymmetric Mo–Ni atom pairs with a shortened interatomic distance of 2.85 Å. This unique structural configuration enables an oxide path mechanism with direct O–O coupling that bypasses traditional scaling relations. Consequently, the catalyst delivers exceptional durability for over 2,000 h at an industrially relevant current density of 3 A cm −2 . When integrated into a laboratory-scale anion-exchange membrane water electrolyser, the anode exhibits low cell voltages of 1.78–1.95 V at 2–3 A cm −2 , alongside more than 1,200 h of stable operation at 3 A cm −2 . To demonstrate commercial viability, we integrate the catalyst into a 71 cm 2 per cell anion-exchange membrane water electrolyser stack, achieving hydrogen production with >99% purity while slashing energy consumption and production costs by 10–17% compared with commercial benchmarks. We further establish a mass-production line for these oxygen evolution reaction electrodes, proving their scalable manufacturing viability and potential to drive cost-effective, zero-emission fuel production at an industrial scale.
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JOURNAL OF NUCLEAR MATERIALS
·
2017
·
IF 2.048
Kuibao Zhang,Dan Yin,Le Peng,Jingjun Wu,Jiali Xue
In this study, zirconolite/Mo composites were rapidly synthesized by a self-propagation reaction that uses MoO 3 as the oxidant accompanied with pressing. Zirconolite is one of the several materials that are being researched as host for lanthanides and actinides in nuclear waste . Nd was used in this study as a surrogate for actinides and was substituted into zirconolite at a stoichiometric ratio to charge balance the Ca and Zr sites (nominal formulation of Ca 1-x Zr 1-x Nd 2x Ti 2 O 7 ). Perovskite , zirconia, and rutile were generated as the minor phases with the addition of Nd 2 O 3 . The XRD results demonstrated that the Nd 2 O 3 loading is approximately 30 wt%. Nd was mainly incorporated into the lattice structure of zirconolite and perovskite. A 42-day leaching test of the Nd-bearing zirconolite/Mo composite showed that the computed normalized leaching rates for Ca and Nd at fairly low values of 9.02 × 10 −2 and 2.10 × 10 −4 g m −2 d −1 , respectively.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Hongda Li,Honggao Deng,Shaonan Gu,Chenpu Li,Boran Tao,Shumin Chen,Xiong He,Guofu Wang,Wenfeng Zhang,Haixin Chang
The “FeMo cofactors” in biological nitrogenase play a decisive role in nitrogen reduction. Herein, a novel bionic Fe/Mo bimetallene was applied in photocatalytic nitrogen reduction. The surface coating Fe/Mo bimetallene of Bi 2 Mo 0.3 W 0.7 O 6 (BMWO) nanocrystals could effectively promote the separation and transportation of photogenerated carriers by multi–electron redox reactions and deliver 2.8 times longer photo–carrier lifetime. Consequently, the nitrogen fixation activity of Fe/Mo bimetallene–coated BMWO nanocrystal photocatalyst was obviously enhanced (218.93 μmol g –1 h −1 ), which was about 4.8 times that of unmodified BMWO nanocrystals. This work provides a novel approach to design bionic Fe/Mo bimetallene–modified inorganic semiconductor photocatalysts for nitrogen reduction.
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Energy Technology
·
2024
·
IF 3.6
Xueli Zhang,Shan Hu,Fangyuan Zhang,Shuchen Xing,Huilin Hu,Jinhua Ye,Defa Wang
As a promising technology to mitigate global carbon emissions, photothermal catalytic CO 2 reduction remains a great challenge in increasing the conversion efficiency and regulating the product selectivity. Herein, a series of phase-separated Ni–Mo alloy catalysts for efficient photothermal CO 2 reduction with tunable CO selectivity is reported. With the increase of Mo content, the evolution rate and selectivity of CO increases. The optimal catalyst Ni 1 Mo 1 achieves 32.1% CO 2 conversion with 98.0% of CO selectivity and 71.1 mmol g cat −1 h −1 of CO evolution rate under a 300 W xenon lamp irradiation. Further increasing the Mo content reduces the CO evolution rate while maintaining the high CO selectivity. In the mechanistic study, it is revealed that the Ni–Mo alloy with an appropriate Ni/Mo ratio (e.g., Ni 1 Mo 1 ) possesses a modified electronic structure with more negative d-band center, which increases the light absorption, reduces the H 2 dissociation, and favors the CO desorption, thereby leading to efficient and selective photothermal reduction of CO 2 to CO. In this work, a viable strategy to design nickel-based catalysts is provided for efficient and selective photothermal CO 2 reduction via composition-mediated modification of electronic structure.
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Junfang Cheng,Zuyu Zhang,Xinyi Li,Zijie Peng,Ziye Feng,Huimin Wang,Sijia Kong,Dawei Liu,Jiantao Zai
The advancement of seawater electrolysis requires highly active and durable nanostructured anode catalysts to enhance the oxygen evolution reaction (OER) while suppressing chloride oxidation (ClOR) and corrosion. High-entropy spinel oxide nanoparticles (HESO NPs) have emerged as promising OER catalysts in alkaline media due to their tunable electronic structures and synergistic multimetal effects. In this study, three nanostructured high-entropy spinel oxides─(CrFeMnNiCo)3O4, (CrFeMnNiCoMo)3O4, and (CrFeMnNiCoRu)3O4─were synthesized via a scalable hydrothermal–calcination method, featuring well-defined spinel phases, uniform elemental distribution, and nanoscale morphology. Notably, the Mo-doped (CrFeMnNiCoMo)3O4 NPs exhibited superior OER performance, achieving low overpotentials of 184 and 229 mV at 10 mA cm–2 in 1 M KOH and alkaline simulated seawater (1 M KOH + 1 M NaCl), respectively, outperforming even the Ru-containing (CrFeMnNiCoRu)3O4 NPs. Furthermore, the nanostructured (CrFeMnNiCoMo)3O4 demonstrated exceptional durability, maintaining stability for 20 h at 50 mA cm–2 in 1 M KOH and 5 h in simulated seawater, significantly surpassing the (CrFeMnNiCo)3O4 NPs. This enhanced stability is attributed to the protective Mo-rich surface layer, which mitigates alkaline corrosion and chloride adsorption. The nanoscale engineering of high-entropy spinel oxides, combined with Mo doping, provides a synergistic strategy to optimize OER activity and ClOR resistance, making them highly suitable for seawater electrolysis applications. This work highlights the potential of high-entropy oxide nanomaterials as efficient and robust electrocatalysts for sustainable hydrogen production.
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Small
·
2022
·Vol. 18
·期 40
·2203835
·
IF 15.153
Shasha Guo,Toshinari Koketsu,Zhiwei Hu,Jing Zhou,Chang-Yang Kuo,Hong-Ji Lin,Chien-Te Chen,Peter Strasser,Lijun Sui,Yu Xie,Jiwei Ma
Transition metal oxides (TMOs) as high-capacity electrodes have several drawbacks owing to their inherent poor electronic conductivity and structural instability during the multi-electron conversion reaction process. In this study, the authors use an intrinsic high-valent cation substitution approach to stabilize cation-deficient magnetite (Fe 3 O 4 ) and overcome the abovementioned issues. Herein, 5 at% of Mo 4+ -ions are incorporated into the spinel structure to substitute octahedral Fe 3+ -ions, featuring ≈1.7 at% cationic vacancies in the octahedral sites. This defective Fe 2.93 ▫ 0.017 Mo 0.053 O 4 electrode shows significant improvements in the mitigation of capacity fade and the promotion of rate performance as compared to the pristine Fe 3 O 4 . Furthermore, physical-electrochemical analyses and theoretical calculations are performed to investigate the underlying mechanisms. In Fe 2.93 ▫ 0.017 Mo 0.053 O 4 , the cationic vacancies provide active sites for storing Li + and vacancy-mediated Li + migration paths with lower energy barriers. The enlarged lattice and improved electronic conductivity induced by larger doped-Mo 4+ yield this defective oxide capable of fast lithium intercalation. This is confirmed by a combined characterization including electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV), galvanostatic intermittent titration technique (GITT) and density functional theory (DFT) calculation. This study provides a valuable strategy of vacancy-mediated reaction to intrinsically modulate the defective structure in TMOs for high-performance lithium-ion batteries.
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