ACS Catalysis
·
2025
·
IF 13.1
Yuanjing Zhang,Guanyi Zhang,Quandong Hou,Shiquan Zhao,Si Wang,Enze Xu,Lei Wang,Xin Zhang,Feng Li,Yusen Yang,Min Wei
Aqueous-phase tandem reactions, as a fundamental aspect of green chemistry, hold a crucial position in the contemporary synthesis of fine chemicals, wherein the advancement of high-performance heterogeneous catalysts remains a formidable challenge. Herein, we report a Pt1Con single-atom alloy (SAA) catalyst in which Pt single atoms are immobilized onto the surface of Co nanoparticles through Pt–Co coordination. The Pt1Con SAA catalyst exhibits a high chemoselectivity for the aqueous-phase hydrogenation–rearrangement reaction of furfural (FAL) to cyclopentanol (CPL) (yield: >93%, considering the carbon loss), with a TOF value of 2257 h–1 (based on Pt). A joint investigation based on reaction dynamics, isotope-label tracing experiments, EPR, and in situ FT-IR verifies a five-step consecutive tandem reaction pathway for the formation of CPL. Notably, during the reaction, the rapid exchange of hydrogen atoms would occur between activated hydrogen species and the water solvent. Furthermore, the water molecule does not serve as a H-donor but is involved in the rearrangement reaction in the side chain of the furan ring. Kinetic studies combined with DFT calculations substantiate that the Pt–Co interface sites effectively lower the energy barrier of the cyclopentanone (CPO) hydrogenation step via facilitating activation adsorption of the carbonyl group, accounting for the largely enhanced catalytic behavior. This study sheds light on the advancement of a highly efficient and stable heterogeneous catalyst for a biomass upgrading reaction in the aqueous phase.
研究领域:
绿色化学
·
催化剂开发
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Lei Liu,Ning Liu,Chengna Dai,Ruinian Xu,Gangqiang Yu,Ning Wang,Biaohua Chen
Realizing MoS2 basal plane activation is highly desirable and challenging in the field of hydrodesulfurization (HDS). Herein, we have developed a new strategy of dual Co single atom doping (SAD) combined with CO in situ regulation, which can successfully activate the basal plane of Co3.6%–MoS2-0.3 generating high ratios of thermostable 1T-plane (∼70%) and large S vacancies. For the first time, a synergistic effect has been unraveled where the lattice substituted neighboring dual SA Co can efficiently activate in-plane S through extensively reducing its band gap (2.21 → 0.14 eV), which tremendously favors S subtraction and 2H → 1T phase transition assisted by CO. Boosted thiophene HDS activity can be eventually achieved with the reaction rate constant (k) being 8.3 times higher than that of commercial cCo3.6%–MoS2 (0.04 → 0.33 h–1). Generally, the present work paves a new way for next-generation HDS catalyst design with activated basal plane.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Materials Today Chemistry
·
2023
·
IF 7.3
W. Tang,L. Zhang,H. Huang,Y. Luo,C. Dong,D. Zhou,A. Li,W. Dong,G. Wang,Y. He
The development of efficient catalysts is essential to promote slow hydrogen reaction kinetics in alkaline solutions. Herein, an ultrathin ZIF-derived efficient HOR/HER electrocatalyst , with Co single-atom-anchored RuCo clusters on N-doped graphitized carbon nanosheets (RuCo/SANC NS), is designed and constructed by a step-by-step calcination strategy. In the RuCo/SANC NS, Co atoms dispersed in carbon nanosheets induce the formation of ultrasmall RuCo clusters and stabilize the RuCo clusters. Abundant coordinatively unsaturated Ru sites are formed on the surface of RuCo clusters due to the small size effect. The electronic structure of the Ru site is regulated by the alloying effect with Co, optimizing the adsorption energy to *H and *OH and accelerating the HER/HOR kinetics. The RuCo/SANC NS catalyst exhibits excellent mass activity with HER of 13.58 A/mg Ru and HOR of 3.85 A/mg Ru , which are about 35.35 and 48.13 times that of Pt/C.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Zhitong Zhou,Weixiang Guan,Xiaoli Pan,Shengxin Zhang,Yang Su,Aiqin Wang,Tao Zhang
Synthesis of primary amines from alcohols is an economical and green route to access high-value N-compounds. However, challenges remain to develop both cost-effective and efficient catalysts. In this study, we developed a Ru-Co/ZrO 2 single-atom alloy catalyst which afforded diverse primary amines from alcohols in the presence of ammonia and hydrogen with exceptional conversion (up to 90%) and selectivity (80%) under mild conditions (0.7 MPa NH 3 , 0.3 MPa H 2 , 160 °C) and exhibited satisfactory stability upon regeneration. The turnover rate was approximately 8.4 times higher than that observed over the Co/ZrO 2 catalyst. Characterizations indicated that the alloyed Ru facilitated the reduction of Co, strengthened the interaction with H 2 and mitigated the over-strong adsorption of aldehyde intermediates. These combined effects contributed significantly to the enhanced catalytic performances. This work presents a promising strategy for the development of advanced catalysts in the amination of alcohols.
研究领域:
催化化学
·
材料化学
·
绿色化学
·
有机合成
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiaoqian Hao,Shengjun Xu,Yan Huang,Shuanglong Ma,Boqiang Gao,Jia Song,Jingzhen Wang,Sihui Zhan
Molybdenum disulfide serves as an ideal support for single atom catalysts (SACs), offering not only coordination elements but also abundant active sites, such as surface defects and vacancies. Herein, a novel Co-SAC (MoSO-Co-C) containing a four-coordinated configuration (Mo-Co-C 3 ) is designed and synthesized, in which the carbon intercalation is utilized to regulate sulfur vacancies for anchoring the Co atom. The introduction of Co atoms and C intercalation significantly enhances the E ads between catalyst and peroxymonosulfate (PMS), favoring the formation of metastable intermediates. The k obs of sulfamethoxazole (SMX) removal for MoSO-Co-C is 9.2 times and 1.8 times higher than those of catalysts without Co or C intercalation. SMX is removed mainly by electron transfer pathway, wherein SMX and PMS act on the same Co site of MoSO-Co-C, and electrons are transferred from SMX to MoSO-Co-C and eventually to PMS. The MoSO-Co-C demonstrated excellent SMX degradation in the diverse water matrices, and the removal efficiency of SMX maintained above 95 % after 72 h of continuous degradation. This study provides new insights into the design of transition metal-based SAC and in-depth understanding of PMS activation mechanism.
研究领域:
环境科学
·
催化
·
水处理
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）