FUEL
·
2023
·
IF 7.4
Junfeng Qin,Qinghui Shen,Cuicui Du,Min Hong,Yixin Yang,Xiaohua Zhang,Jinhua Chen
Heteroatom doping and vacancy engineering play vital roles in designing a high-activity electrocatalyst . Herein, we proposed a novel enriched Se vacancies engineering of the promising ruthenium chalcogenide of RuSe 2 induced by low-valence Cu doping for promoting hydrogen evolution reaction (HER) electrocatalysis in alkaline media. The Cu-doped RuSe 2 with enriched Se vacancies supported on graphitized carbon (Cu-RuSe 2 @C) was synthesized by a simple one-step selenization of bimetallic MOF precursor of Ru/Cu-BTC (1,3,5-benzenetricarboxylic acid) polyhedra. Compared to the Cu(Ⅱ)-dominant doped RuSe 2 (Cu Ⅱ/Ⅰ -RuSe 2 @C) with deficient Se vacancies, the proposed Cu(Ⅰ)-dominant doped RuSe 2 (Cu Ⅰ/Ⅱ -RuSe 2 @C) with enriched Se vacancies exhibited significantly improved electrocatalytic activity, which was potentially derived from the created electron-deficient Ru δ+ and Se ν− sites induced by low-valence Cu doping. Specifically, Cu Ⅰ/Ⅱ -RuSe 2 @C needed only 40 mV overpotential to drive a HER current density of 10 mA cm −2 , comparable to commercial Pt/C (38 mV) and much lower than those of Cu Ⅱ/Ⅰ -RuSe 2 @C (93 mV) and RuSe 2 @C (362 mV). Furthermore, an alkaline Zn-H 2 O fuel cell with a Cu Ⅰ/Ⅱ -RuSe 2 @C cathode was integrated to demonstrate its potential applications, which delivered a maximum power density of 15.1 mW cm −2 and specific capacitance of 660 mAh g −1 with good stability. Two series-connected alkaline Zn-H 2 O cells acted as a chemical energy converter for simultaneous electricity generation and hydrogen coproduction by driving the coupled water splitting.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2021
·Vol. 24
·期 3
·620-627
·
IF 3.545
Wei Zhan,Nan Li,Shixiang Zuo,Zhimin Guo,Chenghong Qiang,Zhengping Li,Jiangquan Ma
The rational design and synthesis of electrocatalysts for hydrogen evolution reaction (HER) remain great challenges. Herein, cubic RuSe2 (c-RuSe2) electrocatalysts with different 1T phase ratios (ranging from 20.53% to 64.97%) and crystallinities (ranging from 1.72% to 89.10%) were developed by a fast and efficient microwave-assisted synthesis method. Remarkably, the c-RuSe2 calcined at 500 °C (RuSe2-500) with 45.46% 1T phase and 86.75% crystallinity exhibited a small overpotential of 29 mV at 10 mA cm−2 and a Tafel slope of 64 mV dec−1, close to the commercial Pt/C (31 mV, 53 mV dec−1) and better than most of the reported materials. The enhanced performance of RuSe2-500 could be attributed to the crystallinity, and the 1T phase content reached a certain equilibrium at 500 °C. Moreover, RuSe2-500 had the smallest charge transfer resistance, mainly due to its abundant active centers and excellent conductivity brought by the 1T phase, which were in favor of the HER kinetics and catalytic performance. This study explored the relationship between the ratio of the 1T phase and crystallinity in c-RuSe2, and gives a new pathway to improve the activity by synergistic regulation.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Yupei Ding,Jie Zhu,Minxia Jiang,Xiaowan Zhan,Jinwen Qin,Xue Jiang,Shuaifeng Wang,Tao Meng,Minhua Cao
RuSe2 has been considered an efficient alkaline hydrogen evolution reaction (HER) electrocatalyst due to its fast water dissociation kinetics and lower price. However, its strong affinity to the adsorbed active intermediates blocks the active sites, hence largely falling short of its full activity potential. Herein, we report a feasible competitive adsorption strategy by introducing oxyphilic molybdenum (Mo) species into RuSe2 (Mo–RuSe2) to regulate the strong interaction between the Ru sites and HER intermediates, enabling highly efficient alkaline HER performance. In situ experimental and theoretical calculation results reveal that the oxyphilic Mo tailoring for RuSe2 can not only alleviate OHad blocking on the Ru sites by the competitive adsorption of OHad between the Ru and Mo sites, but also optimize the hydrogen adsorption Gibbs free energy, thus facilitating the OHad transfer and H2 release process, both of which synergistically promote the regeneration of Ru active sites. The optimized Mo–RuSe2 exhibits an overpotential at 10 mA cm−2 as small as 27 mV and a low Tafel slope of 39 mV dec−1, as well as remarkable long-term stability. This finding is expected to shed new light on developing highly efficient alkaline HER catalysts by regulating the adsorption strength between the active sites and intermediates.
研究领域:
材料科学
·
电化学
·
催化作用
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Fengyue Sun,Wenjing Bao,Chao Feng,Jiahui Bi,Changle Yue,Cong Zhang,Na Liu,Haoyuan Hao,Yukun Lu
The rational design and controllable construction of efficient and stable electrocatalysts is an inevitable trend in sustainable hydrogen production. The transition metal selenides play an important role in the highly active hydrogen evolution reaction (HER) electrocatalysts. Herein, we put forward an “atom-to-cluster” strategy assisted by lacunary polyoxometalates (POMs) to successfully prepare highly dispersed RuSe 2 -WO x @HMCS electrocatalyst. The vacancy-directed effect of lacunary [PW 9 O 34 ] 9− (PW 9 ) was utilized to anchor Ru via coordination bonds and achieve uniform dispersion of Ru at the atomic level. The uniform dispersion of the precursor Ru x [PW 9 O 34 ] (Ru x PW 9 ) at the molecular level was achieved by confining Ru x PW 9 within the mesopores of hollow mesoporous carbon spheres (HMCS). Ultrafine (≈2 nm) and highly dispersed RuSe 2 on WO x was successfully produced at the cluster level by using in situ selenization. Corresponding theoretical calculations demonstrate that the secondary support WO x in combination with RuSe 2 has the synergistic effect in electrocatalytic HER, responding to the significance of trivacant PW 9 . Meanwhile, the conductive support HMCS could promote the exposure of active sites and accelerate electron transfer . Consequently, RuSe 2 -WO x @HMCS exhibited excellent HER activity with overpotentials of only 58 mV and 60 mV at a current density of 10 mA∙cm −2 in 0.5 M H 2 SO 4 and 1 M KOH solutions, respectively. This study provides a feasible “atom-to-cluster” strategy derived from POMs for the modulation and fabrication of low-cost and high-quality HER electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
Journal of Analysis and Testing
·
2019
·Vol. 3
·期 3
·253-259
·
IF 0
Cao Wen,Lin Junshu,Muhammad Faheem,Wang Quan,Wang Xiaoyu,Lou Zhangping,Wei Hui
Nanozyme is a promising field that offers the substitution for natural enzymes using various nanomaterials. Various nanomaterials with peroxidase-like activity were investigated. Among them, transition metal chalcogenides were explored as promising nanozymes due to their excellent enzyme-mimicking activities. However, ruthenium selenide has not been studied as a peroxidase mimic because of the difficulty for synthesis. Herein, we prepared ruthenium selenide nanomaterial with ordered mesoporous structure (P-RuSe 2 ) employing KIT-6 silica as the template. The composition and structure of P-RuSe 2 were fully characterized. Further, its peroxidase-like activity was investigated. P-RuSe 2 possessed excellent peroxidase-mimicking activity, which catalyzed the oxidation of peroxidase substrates, including 3,3′,5,5′-tetramethylbenzidine, o -phenylenediamine, and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) in the presence of H 2 O 2 . Moreover, P-RuSe 2 exhibited higher peroxidase-like activity when compared with several representative nanozymes as well as bulk RuSe 2 . To demonstrate its potential applications, the colorimetric detection systems for H 2 O 2 and glucose were successfully constructed based on P-RuSe 2 nanozyme.
研究领域:
生物化学
·
纳米医学
·
分析化学
✓ 已验证
产品关联
DOI
危险品化学品经营许可证（带存储）