Engineering topics

Jiang, Zhuoli

Publications and source records attributed to Jiang, Zhuoli.

3 records

DOE OSTI2020

Engineering unsymmetrically coordinated Cu-S 1 N 3 single atom sites with enhanced oxygen reduction activity

Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts. Herein, a practical strategy was reported to rationally design single copper atoms coordinated with both sulfur and nitrogen atoms in metal-organic framework derived hierarchically porous carbon (S-Cu-ISA/SNC). The atomic interface configuration of the copper site in S-Cu-ISA/SNC is detected to be an unsymmetrically arranged Cu-S 1 N 3 moiety. The catalyst exhibits excellent oxygen reduction reaction activity with a half-wave potential of 0.918 V vs. RHE. Additionally, through in situ X-ray absorption fine structure tests, we discover that the low-valent Cuprous-S 1 N 3 moiety acts as an active center during the oxygen reduction process. Our discovery provides a universal scheme for the controllable synthesis and performance regulation of single metal atom catalysts toward energy applications.

25 ENERGY STORAGE↗

DOE OSTI2020

In Situ Phosphatizing of Triphenylphosphine Encapsulated within Metal–Organic Frameworks to Design Atomic Co 1 –P 1 N 3 Interfacial Structure for Promoting Catalytic Performance

The engineering coordination environment offers great opportunity in performance tunability of isolated metal single-atom catalysts. For the most popular metal–N x (MN x ) structure, the replacement of N atoms by some other atoms with relatively weak electronegativity has been regarded as a promising strategy for optimizing the coordination environment of an active metal center and promoting its catalytic performance, which is still a challenge. Herein, we proposed a new synthetic strategy of an in situ phosphatizing of triphenylphosphine encapsulated within metal–organic frameworks for designing atomic Co 1 –P 1 N 3 interfacial structure, where a cobalt single atom is costabilized by one P atom and three N atoms (denoted as Co-SA/P-in situ). In the acidic media, the Co-SA/P-in situ catalyst with Co 1 –P 1 N 3 interfacial structure exhibits excellent activity and durability for the hydrogen evolution reaction (HER) with a low overpotential of 98 mV at 10 mA cm –2 and a small Tafel slope of 47 mV dec –1 , which are greatly superior to those of catalyst with Co 1 –N 4 interfacial structure. We discover that the bond-length-extended high-valence Co 1 –P 1 N 3 atomic interface structure plays a crucial role in boosting the HER performance, which is supported by in situ X-ray absorption fine structure (XAFS) measurements and density functional theory (DFT) calculation. With this work, we hope to promote the development of high performance metal single-atom catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions

The regulation of catalytic activity in the oxygen reduction reaction (ORR) is significant to the development of metal–air batteries and other oxygen involving energy conversion devices. Herein, we propose an atomic interface strategy to construct a single atom copper catalyst (denoted as Cu-SA/SNC) which exhibits enhanced ORR activity with a half-wave potential of 0.893 V vs. RHE in alkaline media. Moreover, synchrotron-radiation-based X-ray absorption fine structure (XAFS) investigations together with density functional theory (DFT) calculations reveal that the isolated bond-shrinking low-valence Cu (+1)–N 4 –C 8 S 2 atomic interface moiety serves as an active site during the ORR process, and the synergistic mechanism between the Cu species and the carbon matrix at the atomic interface plays a critical role in boosting the ORR efficiency, by adjusting the reaction free energy of intermediate adsorption. Furthermore, this atomic interface concept may provide an alternative methodology for the rational design of advanced oxygen electrode materials and new probability to improve their catalytic performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗