Catalysts
·
2023
·Vol. 13
·期 7
·1103
·
IF 3.9
Jinfeng Tian,Xing Wen,Wenfeng Hu,Li Luo,Wei Wang,Keying Lin,Haijuan Zhan,Baojun Ma
As non-noble metal co-catalysts, Nitrides have received extensive attention for their high efficiency and low cost in photocatalytic hydrogen production. In this study, we develop a novel composite co-catalyst of Au/Ta3N5that significantly enhanced the photocatalytic hydrogen production activity of CdS. The activity of photocatalyst (Au/Ta3N5)/CdS is 7.3 times of bare CdS and 2.2 times of Ta3N5/CdS. The proper capacitance and enhanced activity of Ta3N5demonstrates the capacitance catalysis effect of Ta3N5, which improves the charges separation and storing of the photoexcited electrons from CdS. Au acts as an active site for proton reduction to further improve the activity.Keywords:co-catalyst;Ta3N5;capacitance catalysis;photocatalytic hydrogen production
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xiaoqiang Zhan,Deliu Ou,Yapeng Zheng,Bing Li,Leyao Xu,Hongli Yang,Wenxiang Yang,Haitao Zhang,Huilin Hou,Weiyou Yang
Currently, two-dimensional/two-dimensional (2D/2D) van der Waals heterojunctions, as novel and excellent candidates for photocatalysts, have attracted significant attention because of their fundamentally improved interfacial charge separation/transfer and massive reactive centers. Herein, novel 2D/2D Ta 3 N 5 -nanosheet/ReS 2 -nanosheet van der Waals heterojunction photocatalysts are rationally designed through a method combining template-assisted and solution-adsorption processes. The resultant heterojunctions exhibit enhanced interfacial charge transfer, boosted light absorption and significantly increased reaction sites for hydrogen evolution. Correspondingly, they deliver a high photocatalytic hydrogen production activity of 615 μmol g −1 h −1 , which is ∼3 and ∼12 times greater than that of bare Ta 3 N 5 nanosheets and ReS 2 nanosheets, respectively, and superior to those in the most recent reports about photocatalytic water splitting on Ta 3 N 5 material, implying their potential applications as advanced catalysts for hydrogen evolution.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 35
·13176-13183
·
IF 4.052
Lang Pei,Yongjun Yuan,Jiasong Zhong,Taozhu Li,Tao Yang,Shicheng Yan,Zhenguo Ji,Zhigang Zou
Tantalum nitride (Ta3N5) with an appealing band gap (∼2.1 eV) has emerged as a promising catalyst in the photocatalysis field. However, Ta3N5 application in the photocatalytic hydrogen evolution reaction (HER) is limited due to disadvantages such as unsatisfactory separation and transfer of photogenerated carriers. Here we utilize MoS2 as co-catalysts to promote the kinetics of photocatalytic H2 evolution over Ta3N5. The Ta3N5 nanorods were encapsulated into 3D hydrangea-like MoS2 for maximizing the contact areas between Ta3N5 and MoS2 and offering rich active sites. More importantly, spectroscopic analysis and theoretical calculations consistently reveal that the unique interfacial interaction, as well as the matching band alignment between Ta3N5 and MoS2, accelerates the photogenerated charge extraction from Ta3N5 to MoS2, reducing charge recombination losses in Ta3N5. Thus, the optimized Ta3N5/MoS2 hybrid exhibits a substantially enhanced hydrogen evolution rate (56.5 μmol h−1), over 22 times higher than that of pristine Ta3N5. This work may provide a general strategy to overcome the low photocatalytic activity of nitrides for hydrogen evolution.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Zirui Lou,Yingchen Yang,Yichen Wang,Chao Qin,Rong Liang,Yanwen Wang,Zhizhen Ye,Liping Zhu
Ta 3 N 5 is a promising candidate for photoelectrochemical (PEC) water splitting. Recently gratifying photocurrents have been reported through various advanced techniques. However, obtaining high performance Ta 3 N 5 photoanode prepared by direct oxidation and nitridation remains challenging. In this work, efficient Ta 3 N 5 photoanode was fabricated on Ta foil by direct oxidation and nitridation method with LaCl 3 flux mediated treatment. The highest photoresponse (8.2 mA cm −2 @ 1.23 V RHE ) for direct oxidized and nitrided Ta 3 N 5 is achieved with the help of LaCl 3 flux, which is nearly doubled compared to the untreated counterparts. Theoretical analysis suggests an interfacial charge transfer in LaTaON 2 /Ta 3 N 5 heterostructure and significant increase in carrier concentration on La doped Ta 3 N 5 surface. The introduction of LaCl 3 flux brings a new look to this traditional method and it may potentially be applied to large area and low cost photoanodes.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Lang Pei,Xusheng Wang,Heng Zhu,He Yu,Sateesh Bandaru,Shicheng Yan,Zhigang Zou
Photothermal catalysis, which combines light promotion and thermal activation, is a promising approach for converting CO2 into fuels. However, the development of photothermal catalysts with effective light-to-heat conversion, strong charge transfer ability, and suitable active sites remains a challenge. Herein, the photothermal effect- and interfacial N–Ni/Ta–O bond-modulated heterostructure composed of oxygen vacancy-rich NiOx and Ta3N5 was rationally fabricated for efficient photothermal catalytic CO2 reduction. Beyond the charge separation capability conferred by the NiOx/Ta3N5 heterojunction, we observed that the N–Ni and Ta–O bonds linking NiOx and Ta3N5 form a spatial charge transfer channel, which enhances the interfacial electron transfer. Additionally, the presence of surface oxygen vacancies in NiOx induced nonradiative relaxation, resulting in a pronounced photothermal effect that locally heated the catalyst and accelerated the reaction kinetically. Leveraging these favorable factors, the NiOx/Ta3N5 hybrids exhibit remarkably elevated activity (≈32.3 μmol·g–1·h–1) in the conversion of CO2 to CH4 with near-unity selectivity, surpassing the performance of bare Ta3N5 by over 14 times. This study unveils the synergistic effect of photothermal and interfacial chemical bonds in the photothermal–photocatalytic heterojunction system, offering a novel approach to enhance the reaction kinetics of various catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Guoan Lin,Chi Zhang,Xiaoxiang Xu
Charge separation is generally considered as the most critical step to achieve efficient photocatalytic reactions. Although charge separation can be promoted by a semiconductor heterojunction, its efficacy is inherently restrained by the mismatched atomic arrangements across the heterojunction interfaces. Here, Ta 3 N 5 –LaTaON 2 heterojunction with matched interfaces has been fabricated by one-step ammonolysis treatment of KLaTa 2 O 7 . The match interfaces are formed by nearly perfect adhesion of Ta 3 N 5 (010) and LaTaON 2 (10 1 ¯ ) facets whose interatomic distance is similar. Compared with conventional heterojunction, the so-formed Ta 3 N 5 –LaTaON 2 heterojunction are extremely efficient in accelerating charge separation which in turn enables a high photocatalytic activity. An apparent quantum efficiency as high as 11.6% at 420 ± 20 nm has been reached by Ta 3 N 5 –LaTaON 2 heterojunction, which is almost three times higher than Ta 3 N 5 /LaTaON 2 mixtures. These results signify the importance of matched heterojunction interfaces for charge separation and provide a paradigm in the design of efficient heterojunction-based semiconductor photocatalysts.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 151
·期 6
·1728-1737
·
IF 2.482
Huang Huiting,Shen Lijuan,Yang Shuai,Hu Wenjian,Zhang Lili,Feng Jianyong,Jiang Lilong,Yu Tao,Li Zhaosheng,Zou Zhigang
Abstract In addition to traditional metal oxides, N-containing compound would become efficient catalyst for H 2 S selective oxidation. TaON and Ta 3 N 5 , taking as examples, with porous structure are able to selectively oxidize H 2 S into sulfur. TaON exhibits ca. 99% H 2 S conversion and ca. 89% sulfur selectivity at 250 ℃, while Ta 3 N 5 exhibits near complete H 2 S conversion (~ 100%) and 86% sulfur selectivity at 250 ℃. TaON of lower N content shows higher sulfur selectivity (~ 90–100%) above 130 ℃, compared with that (~ 86–95%) over Ta 3 N 5 . Whereas, Ta 3 N 5 of higher N content demonstrates higher H 2 S conversion (~ 30–40%) below 160 ℃, compared with that (~ 6–30%) over TaON. Temperature programmed desorption results show that Ta 3 N 5 owns larger amount of acid sites and weaker basic sites than TaON. Over Ta 3 N 5 , the reactant molecules could dissociatively adsorb on acid sites more frequently and could be easier to move across the weaker basic sites, thus increasing probability for reaction at low temperature. Manipulating both cations and anions in N-containing compound can alter surface property for optimization of selective H 2 S oxidation. Graphic Abstract
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Xiao Yequan,Fan Zeyu,Nakabayashi Mamiko,Li Qiaoqiao,Zhou Liujiang,Wang Qian,Li Changli,Shibata Naoya,Domen Kazunari,Li Yanbo
The trade-off between light absorption and carrier transport in semiconductor thin film photoelectrodes is a major limiting factor of their solar-to-hydrogen efficiency for photoelectrochemical water splitting. Herein, we develop a heterogeneous doping strategy that combines surface doping with bulk gradient doping to decouple light absorption and carrier transport in a thin film photoelectrode. Taking La and Mg doped Ta 3 N 5 thin film photoanode as an example, enhanced light absorption is achieved by surface La doping through alleviating anisotropic optical absorption, while efficient carrier transport in the bulk is maintained by the gradient band structure induced by gradient Mg doping. Moreover, the homojunction formed between the La-doped layer and the gradient Mg-doped layer further promotes charge separation. As a result, the heterogeneously doped photoanode yields a half-cell solar-to-hydrogen conversion efficiency of 4.07%, which establishes Ta 3 N 5 as a leading performer among visible‐light‐responsive photoanodes. The heterogeneous doping strategy could be extended to other semiconductor thin film light absorbers to break performance trade-offs by decoupling light absorption and carrier transport.
研究领域:
材料科学
·
光电化学
·
可再生能源
✓ 已验证
DOI
高影响因子
Energy & Environmental Science
·
2013
·Vol. 6
·期 11
·3322-3330
·
IF 11.653
Jungang Hou,Zheng Wang,Chao Yang,Huijie Cheng,Shuqiang Jiao,Hongmin Zhu
Ta3N5 nanorod arrays were fabricated by nitridation of fluorine-containing tantalum oxide (F–Ta2O5) nanorod arrays grown in situ on Ta substrates by a one-pot vapour-phase hydrothermal induced self-assembly technique. In this protocol, the in situ generation and the morphology of arrays elaborately adjusted by reaction time, play a vital role in the formation of the F–Ta2O5 nanorod arrays and a highly conductive interlayer between the nanorods and the substrate. Due to the shape anisotropy, ordered hierarchical structure and high surface area, a high photoelectrochemical activity was achieved by the optimum Ta3N5 nanorod photoelectrode with a photocurrent density of 1.22 mA cm−2 under AM 1.5G irradiation at 1.23 V vs. RHE (reversible hydrogen electrode). Furthermore, a higher and more stable photocurrent was demonstrated by combining the highly active Ta3N5 nanorods with stable Co3O4/Co(OH)2 (Co3O4/Co(II)) bilayer catalysts when compared with that demonstrated for Co(II)/Ta3N5 and Co3O4/Ta3N5 photoelectrodes, exhibiting that not only is the onset potential negatively shifted but also the photocurrent and the stability are significantly improved, which is correlated to an order of magnitude reduction in the resistance to charge transfer at the Ta3N5/H2O interface. Specifically, about 92% of the initial stable photocurrent remains after long-term irradiation at 1.23 V vs. RHE. At 1.23 V vs. RHE, the photocurrent density of Co3O4/Co(II)/Ta3N5 arrays reached 3.64 mA cm−2 under AM 1.5G simulated sunlight at 100 mW cm−2, and a maximum IPCE of 39.5% was achieved at 440 nm. This combination of catalytic activity, stability, and conformal decoration makes this a promising approach to improve the photoelectrochemical performance of photoanodes in the general field of energy conversion.
研究领域:
材料科学
·
能源转换
·
催化化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 38
·20439-20447
·
IF 8.867
Lang Pei,Zhe Xu,Zhan Shi,Heng Zhu,Shicheng Yan,Zhigang Zou
Charge separation/transfer and photocorrosion are two major factors limiting the photoelectrochemical (PEC) applications of the Ta3N5 photocatalyst. Herein, we have fabricated Ta3N5 single-crystal nanorods with Mg doping by flux-assisted crystal growth, aiming to shorten the charge transport distance and increase the electrical conductivity. The optimized Mg-doped Ta3N5 photoanodes exhibit an unprecedented PEC water splitting activity with an AM 1.5G photocurrent of 1.5 mA cm−2 at 1.23 VRHE. The high performance is attributed to the fact that the bulk modification, Mg doping, can induce oxygen-impurity surface states as effective electron trap centers, thus increasing the electrical conductivity of Ta3N5 and charge separation efficiency. After a conformal surface modification with CoOOH by a simple electrodeposition method as a water oxidation electrocatalyst to improve the hole extraction and reaction kinetics, the Mg-doped Ta3N5 photoanodes afford an over 4-fold increase in photocurrent (ca. 6.5 mA cm−2 at 1.23 VRHE) and about 70% retention of the initial photocurrent after 70 min irradiation at 1.0 VRHE. Our results testify that the bulk and surface co-modification is an effective route to develop high-performance PEC water splitting devices.
研究领域:
材料科学
·
能源科学
·
表面化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 77
·62519-62526
·
IF 3.84
Wen Wang,Hua-Bin Fang,Yan-Zhen Zheng,Yanke Che,Xia Tao,Jian-Feng Chen
A novel 3D p–n heteroarchitecture Ag3PO4/Ta3N5 composite photocatalyst with double visible-light-response characteristics has been prepared using an in situ template-free precipitation method. It is found that the fascinating Ag3PO4/Ta3N5 exhibited high superior photoactivity and photostability compared to bare Ag3PO4 and Ta3N5 for the degradation of RhB under visible light irradiation. The improved performance of the composite is primarily attributable to sufficient visible-light harvesting, efficient charge separation and transfer of photogenerated electrons and holes resulting from matched energy bandgaps and sufficient p–n hetero-interfaces between Ag3PO4 and Ta3N5. The quenching effects of different scavengers demonstrate that the reactive h+ and O2−˙ species played a major role in the photodegradation process. It is expected that the 3D p–n heterostructure composite fabricated via a facile precipitation method, may be a promising candidate for organic pollutant degradation.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Catalysis
·
2020
·Vol. 3
·期 11
·932-940
·
IF 30.471
Xiao Yequan,Feng Chao,Fu Jie,Wang Faze,Li Changli,Kunzelmann Viktoria F.,Jiang Chang-Ming,Nakabayashi Mamiko,Shibata Naoya,Sharp Ian D.,Domen Kazunari,Li Yanbo
Ta 3 N 5 is a promising photoanode material with a theoretical maximum solar conversion efficiency of 15.9% for photoelectrochemical water splitting. However, the highest applied bias photon-to-current efficiency achieved so far is only 2.72%. To bridge the efficiency gap, effective carrier management strategies for Ta 3 N 5 photoanodes should be developed. Here, we propose to use gradient Mg doping for band structure engineering and defect control of Ta 3 N 5 . The gradient Mg doping profile in Ta 3 N 5 induces a gradient of the band edge energetics, which greatly enhances the charge separation efficiency. Furthermore, defect-related recombination is significantly suppressed due to the passivation effect of Mg dopants on deep-level defects and, more importantly, the matching of the gradient Mg doping profile with the distribution of defects within Ta 3 N 5 . As a result, a photoanode based on the gradient Mg-doped Ta 3 N 5 delivers a low onset potential of 0.4 V versus that of a reversible hydrogen electrode and a high applied bias photon-to-current efficiency of 3.25 ± 0.05%.
研究领域:
材料科学
·
光电化学
·
半导体物理
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）