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学者姓名：刘储浩
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Abstract ：
Undercoordinated sites on metal catalysts are pivotal for enhancing electrocatalytic reactions, particularly in processes like coreduction, where multiple intermediates must be generated and coupled. Traditional synthesis methods, however, are limited in their ability to produce these low-coordination sites. In this study, we developed an amorphous indium catalyst (A-In@BO x ) using a boron oxide-assisted method that achieves a uniquely low coordination number (CN = 3.6) with a high density of 67.2 wt %. This structural characteristic significantly enhances the catalytic efficiency for urea synthesis, achieving a yield rate of 2317.58 mu g h-1 mgcat -1 and a Faradaic efficiency of 51.43% at -0.45 V versus RHE. The undercoordinated indium sites (UC-In) on A-In@BO x improve the conversion of NO3 - to NO2 -, effectively generating *NO2 as a crucial nitrogen intermediate for carbon-nitrogen coupling, while the inherently limited activity for CO2 reduction maintains *CO2 as the primary carbon intermediate. Our integrated in situ spectroscopy and theoretical simulations show that electron transfer from UC-In to *NO2 markedly reduces the free energy barrier for CO2 protonation from 1.77 to 0.04 eV, thus promoting the formation of the key *COOH-NO2 intermediate. This breakthrough not only offers a fresh pathway for optimizing urea synthesis but also elucidates the coreduction mechanisms at undercoordinated metal sites, paving the way for the design of highly selective catalysts.
Keyword ：
amorphous amorphous carbon-nitrogencoupling carbon-nitrogencoupling electrocatalytic urea synthesis electrocatalytic urea synthesis high-density activesites high-density activesites low coordination low coordination
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| GB/T 7714 | Liu, Chuhao , Yang, Tongtong , Li, Shiyun et al. Amorphization Induces High-Density Undercoordinated Indium Sites for Enhanced Electrocatalytic Urea Synthesis [J]. | ACS CATALYSIS , 2025 , 15 (10) : 8489-8496 . |
| MLA | Liu, Chuhao et al. "Amorphization Induces High-Density Undercoordinated Indium Sites for Enhanced Electrocatalytic Urea Synthesis" . | ACS CATALYSIS 15 . 10 (2025) : 8489-8496 . |
| APA | Liu, Chuhao , Yang, Tongtong , Li, Shiyun , Wu, Yue , Jiang, Qinyu , Xie, Jisheng et al. Amorphization Induces High-Density Undercoordinated Indium Sites for Enhanced Electrocatalytic Urea Synthesis . | ACS CATALYSIS , 2025 , 15 (10) , 8489-8496 . |
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Abstract ：
In this study, we encapsulated Bi in hollow carbon spheres to form a nanoreactor. It shows good activation ability for CO2 and NO3-, and significantly enhances the coupling of C-N intermediates. This improves urea selectivity by 66% compared to unencapsulated Bi-based catalysts and shows good stability.
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| GB/T 7714 | Wu, Yue , Zhang, Bozhao , Yu, Yuan et al. Boosting small-molecule reduction with bismuth-based nanostructured reactors [J]. | CHEMICAL COMMUNICATIONS , 2025 , 61 (58) : 10800-10803 . |
| MLA | Wu, Yue et al. "Boosting small-molecule reduction with bismuth-based nanostructured reactors" . | CHEMICAL COMMUNICATIONS 61 . 58 (2025) : 10800-10803 . |
| APA | Wu, Yue , Zhang, Bozhao , Yu, Yuan , Jiang, Qinyu , Feng, Shanru , Lin, Yongjin et al. Boosting small-molecule reduction with bismuth-based nanostructured reactors . | CHEMICAL COMMUNICATIONS , 2025 , 61 (58) , 10800-10803 . |
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Abstract ：
Electrocatalytic nitrate reduction is an attractive route for sustainable hydroxylamine synthesis, but its selectivity is limited by over-reduction and competing hydrogen evolution, highlighting the need for in-depth mechanistic understanding to guide catalyst design. Here, we systematically investigate the electrochemical synthesis of hydroxylamine via a formaldehyde-mediated method on titanium oxides. An electrochromic rutile array prepared via a wet-chemical route achieved a Faradaic efficiency (FE) of 92.6% (for formaldehyde oxime) and a corresponding yield rate of up to 2085 mu mol cm-2 h-1 under ambient conditions. Mechanistic studies reveal that the electrochromism is a macroscopic manifestation of the protonation of Ob (bridging oxygen) sites and the formation of Ov (oxygen vacancies) and Ti3+, which act as proton "sponges" and electron reservoirs. Formaldehyde not only serves as the capturing agent but also helps to stabilize *NH2OH through molecular tuning, thereby achieving high selectivity. Through formaldehyde-nitrate electro-reforming, hydrogen, formic acid, and hydroxylamine can be coproduced at 200 mA cm-2 under an ultralow cell voltage of 0.78 V. This work links the catalytic performance of hydroxylamine electrosynthesis to the dynamic surface of titanium oxides, offering insights into selectivity control in nitrate electroreduction and providing a green, cost-effective alternative to conventional hydroxylamine synthesis.
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| GB/T 7714 | Zhang, Jiaqi , Zhao, Erbo , Hsueh, Chou-Hung et al. Electrochromic Rutile with Dynamically Tailored Surfaces in Formaldehyde-Mediated Hydroxylamine Electrosynthesis [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (24) : 20559-20570 . |
| MLA | Zhang, Jiaqi et al. "Electrochromic Rutile with Dynamically Tailored Surfaces in Formaldehyde-Mediated Hydroxylamine Electrosynthesis" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 24 (2025) : 20559-20570 . |
| APA | Zhang, Jiaqi , Zhao, Erbo , Hsueh, Chou-Hung , Cheong, Weng-Chon Max , Tan, Xin , Liu, Chuhao et al. Electrochromic Rutile with Dynamically Tailored Surfaces in Formaldehyde-Mediated Hydroxylamine Electrosynthesis . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (24) , 20559-20570 . |
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Cocatalyst is of paramount significance to provide fruitful active sites for suppressing the spatial charge recombination toward boosted photocatalysis. Up to date, exploration of robust and stable cocatalysts is remained challenging. Inspired by the intrinsic merits of single-atom catalysts (SACs), such as distinctive electronic structure and high atomic utilization efficiency, single-atom/transition metal chalcogenides (TMCs) is utilized as a model to synthesize CdS-Pd single-atom catalyst (CdS-PdSA) heterostructures. This demonstrates the precise anchoring of isolated metal single-atom catalysts (SACs) onto TMCs through a simple yet effective wet-chemical strategy. The resulting heterostructures exhibit significantly enhanced and stable photocatalytic activity for selective anaerobic organic transformations and hydrogen production under visible light. This enhancement is primarily inferred due to the role of Pd SACs as electron pumps, which directionally trap the electrons photoexcited over CdS, accelerating the spatial charge separation and prolonging the carrier lifespan. The charge transport route and photocatalytic mechanism are elucidated. This work underscores the potential of SACs as cocatalysts in heterogeneous photocatalysis, offering valuable insights for the rational design of atomic-level cocatalysts for solar-to-chemical energy conversion and beyond. Metal single atoms act as electron pumps to expedite the unidirectional electron transfer from the TMCs matrix to the metal single atoms, contributing to the markedly augmented organic transformation and hydrogen generation activities. image
Keyword ：
charge transfer charge transfer electron pump electron pump photoreduction catalysis photoreduction catalysis single atoms single atoms TMC TMC
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| GB/T 7714 | Chen, Jia-Qi , Cai, Yu-Shan , Yan, Xian et al. Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis [J]. | SMALL , 2024 , 20 (51) . |
| MLA | Chen, Jia-Qi et al. "Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis" . | SMALL 20 . 51 (2024) . |
| APA | Chen, Jia-Qi , Cai, Yu-Shan , Yan, Xian , Mo, Qiao-Ling , Yuan, Jiao-Nan , Liu, Chu-Hao et al. Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis . | SMALL , 2024 , 20 (51) . |
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