Zhitan Wu

National University of Singapore

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Quan‐Hong Yang

State Key Laboratory of Chemical Engineering

Ying Tao

Shanghai Jiao Tong University

Kian Ping Loh

National University of Singapore

Tongxin Shang

Nantong University

Yaqian Deng

First Affiliated Hospital of Shihezi University Medical College

Shuhe Han

Hong Kong Polytechnic University

Hai‐Sen Xu

Sun Yat-sen University

Yijia Yuan

Jilin University

Derong Chen

Beijing Institute of Technology

Junhao Lin

Southern University of Science and Technology

Cooperative Institutions

Tianjin University

National University of Singapore

Collaborative Innovation Center of Chemical Science and Engineering Tianjin

Unité Matériaux et Transformations

State Key Laboratory of Chemical Engineering

Chinese Academy of Sciences

Tsinghua University

University of Chinese Academy of Sciences

Tsinghua–Berkeley Shenzhen Institute

Shanghai Jiao Tong University

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A bio-derived sheet-like porous carbon with thin-layer pore walls for ultrahigh-power supercapacitors

Nano Energy (2020)

Tongxin Shang Yue Xu Pei Li Junwei Han Zhitan Wu

Tortuosity

Carbon fibers

Power density

10.1016/j.nanoen.2020.104531

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Citations (203)

Boosting C2+ Alcohols Selectivity and Activity in High‐Current CO Electroreduction using Synergistic Cu/Zn Co‐Catalysts

Angewandte Chemie International Edition (2024)

Zhitan Wu Nannan Meng Rong Yang Maoxin Chen Jinhui Pan

The electrosynthesis of multi-carbon (C2+) alcohols, specifically ethanol and n-propanol through CO electroreduction (CORR) in H2O, presents a sustainable pathway for intermittent renewable energy storage and a low-carbon economy. However, achieving high selectivity for alcohol production at industrial current densities is kinetically hampered by side reactions such as ethylene generation and hydrogen evolution reaction, which result from competing adsorption of *CO and *H. In this study, we developed a Cu/Zn alloy catalyst to simultaneously enhance the activity and selectivity for alcohol production by increasing CO capture capacity and enriching active hydrogen on Cu sites. Our findings demonstrate that the Cu/5Zn alloy with a molar ratio of Cu to Zn of 95:5 exhibits a Faradaic efficiency of 50% for the selective electrosynthesis of C2+ alcohols during ampere-level CO electrolysis. Mechanistic investigations revealed that the Cu/Zn alloy promotes polarized Cu sites, enhancing CO adsorption while facilitating the spillover of hydrogen atoms from Zn to Cu sites, contributing to selective alcohol formation.

Boosting

10.1002/anie.202420283

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Assembling of MXenes from Liquid to Solid, Including Liquid Crystals, Fibers

Long Yu Zhitan Wu Ying Tao Quan‐Hong Yang

Assembly of MXenes from the liquid phase into solid macrostructures brings important opportunities to construct functionalized MXene materials with the desired structure for applications in diverse fields. Due to their intrinsic flexibility and hydrophilicity, MXenes can be directly assembled from MXene colloidal solution by diverse solution-processed assembly techniques, which provides a simple and effective way to produce MXene-based macroscopic architectures, mainly including three kinds of dimensionality varied materials, named 1D fibers, 2D films, and 3D hydrogel or aerogels. This chapter starts with a brief overview of these MXene-based macroscopic assemblies, then these macroforms are introduced by dividing them into pure and composite assemblies with emphasis on their structural features as well as assembly strategies and mechanisms; the potential applications are also discussed, including conductive transparent coatings, electrochemical energy storage, drug delivery, sensing, and electromagnetic interference shielding. Finally, we offer insights into the prospects and the challenges ahead for rational design and controlled preparation of macroscopic MXene-based functional materials from solution.

MXenes

10.1002/9781119869528.ch15

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MXene-assisted polymer coating from aqueous monomer solution towards dendrite-free zinc anodes

Journal of Energy Chemistry (2022)

Ning Wang Zhitan Wu Long Yu Derong Chen Chuannan Geng

10.1016/j.jechem.2022.06.009

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Citations (46)

Ion-Conductive Metallo-Covalent Organic Frameworks Constructed with Tridentate Ligand and Zn Nodes

Journal of the American Chemical Society (2023)

Fangzheng Chen Kun Zhang Yijia Yuan Walter P. D. Wong Gang Wang

Metallo-covalent organic frameworks (metallo-COFs) are organometallic scaffolds in which covalently bonded organic frameworks are interwoven with metal-coordinated pendant groups. Unlike the rigid ligands traditionally used for metal coordination, the utilization of "soft" ligands allows for configurable topology and pore structure in metallo-COFs, particularly when the ligands are generated in situ during dynamic synthesis. In this study, we present the rational synthesis of metallo-COFs based on pyridine-2,6-diimine (pdi), wherein the incorporation of Zn2+ ions and in situ-generated tridentate ligands (pdi) yields metallo-COFs with a square-like lattice. In the absence of Zn2+ ions, a topological isomer COF with a Kagome lattice is instead produced. Thus, the presence or absence of Zn2+ ions allows us to switch between two distinct morphologies corresponding to metallo-COF or COF. In comparison to Brønsted acid-catalyzed COF, which necessitates postmetallization for loading metal ions, the metal-templated COF synthesis method yields COFs with improved crystallinity and approximately 1:1 [Zn2+]/ligand composition. Building upon the metal-templated COF synthesis approach, we successfully synthesized pdiCOF-Zn-2 and pdiCOF-Zn-3, which possess square-like and honeycomb lattices, respectively. The enhanced crystallinity and near 1:1 [Zn2+]/ligand composition of pdiCOF-Zn-3 (honeycomb) facilitate its application as ion transport channels.

Diimine

10.1021/jacs.3c09114

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Dynamically Stable Cu0Cuδ+ Pair Sites Based on In Situ‐Exsolved Cu Nanoclusters on CaCO3 for Efficient CO2 Electroreduction

Angewandte Chemie International Edition (2025)

Rongrong Zhang Haibin Ma Shuhe Han Zhitan Wu Xin Zhou

Copper‐based catalysts are the choice for producing multi‐carbon products (C2+) during CO2 electroreduction (CO2RR), where the Cu0Cuδ+ pair sites are proposed to be synergistic hotspots for C‐C coupling. Maintaining their dynamic stability requires precise control over electron affinity and anion vacancy formation energy, posing significant challenges. Here, we present an in‐situ reconstruction strategy to create dynamically stable Cu0Cu0.18+OCa motifs at the interface of exsolved Cu nanoclusters and CaCO₃ nanospheres (Cu/CaCO₃). In‐situ XAFS analysis confirmed the low‐valency state of Cuδ+ during CO2RR. DFT calculations demonstrated that the nanocluster size arises from the balance between metal‐support interactions and Cu‐Cu cohesive energy, while the dynamic stability of rich interfacial Cuδ+ sites is attributed to their low electron affinity and high CO32‐ vacancy formation energy, which collectively contribute to reduced reducibility. The transformed Cu/CaCO₃ exhibits an impressive C2+ Faradaic efficiency of 83.7% at a partial current density of 393 mA cm‐2, facilitated by adsorption of *CO with varying electronegativity at heterogeneous copper sites that lowers the C‐C coupling energy barrier. Our findings establish insoluble carbonate as an effective anion pairing for Cu0Cuδ+ sites, highlighting the effectiveness of the in‐situ reconstitution strategy in producing a high density of dynamically stable Cu0Cuδ+ pair sites.

Nanoclusters

10.1002/anie.202421860

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CCDC 2303276: Experimental Crystal Structure Determination

The Cambridge Structural Database (2023)

Fangzheng Chen Kun Zhang Yijia Yuan Walter P. D. Wong Gang Wang

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

10.5517/ccdc.csd.cc2h9r7t

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High yield electrosynthesis of oxygenates from CO using a relay Cu-Ag co-catalyst system

Nature Communications (2024)

Nannan Meng Zhitan Wu Yanmei Huang Jie Zhang Maoxin Chen

Abstract As a sustainable alternative to fossil fuel-based manufacture of bulk oxygenates, electrochemical synthesis using CO and H 2 O as raw materials at ambient conditions offers immense appeal. However, the upscaling of the electrosynthesis of oxygenates encounters kinetic bottlenecks arising from the competing hydrogen evolution reaction with the selective production of ethylene. Herein, a catalytic relay system that can perform in tandem CO capture, activation, intermediate transfer and enrichment on a Cu-Ag composite catalyst is used for attaining high yield CO-to-oxygenates electrosynthesis at high current densities. The composite catalyst Cu/30Ag (molar ratio of Cu to Ag is 7:3) enables high efficiency CO-to-oxygenates conversion, attaining a maximum partial current density for oxygenates of 800 mA cm −2 at an applied current density of 1200 mA cm −2 , and with 67 % selectivity. The ability to finely control the production of ethylene and oxygenates highlights the principle of efficient catalyst design based on the relay mechanism.

Oxygenate

Electrosynthesis

10.1038/s41467-024-48083-w

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Citations (2)

A Gelation‐Assisted Approach for Versatile MXene Inks

Advanced Functional Materials (2022)

Derong Chen Long Yu Zhitan Wu Ximan Dong Ning Wang

Abstract Due to outstanding electrical conductivity and excellent solution processing ability, MXenes show great potential as inks for printed/coated electronic devices. To meet the rheological requirements, an ultra‐high concentration is usually involved to formulate MXenes into versatile inks, however, low efficiency in rheology regulation, and restacking issues of MXene sheets hinder their further applications. Herein, a gelation‐assisted approach is proposed to prepare versatile MXene inks with a 3D interlinked network to well address above issues. With an effective combination of cross‐linking as well as the swelling of interlinked network, the gel ink exhibits tunable rheological properties by simply tuning the water amount within the sol‐gel system. Among various applicable printing/coating techniques ranging from painting to extrusion printing, blade coating is selected to demonstrate the advantage of MXene gel ink. The smooth coating layer with interlinked 3D structures is greatly beneficial to the uniform and dense zinc deposition with high reversibility, and endows the aqueous zinc ion batteries with a remarkable rate capability. This work provides an alternative approach to prepare versatile MXene inks and would offer MXenes new opportunities for their application in advanced printable electronic devices.

MXenes

10.1002/adfm.202204372

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Citations (28)

CCDC 2289655: Experimental Crystal Structure Determination

The Cambridge Structural Database (2023)

Fangzheng Chen Kun Zhang Yijia Yuan Walter P. D. Wong Gang Wang

10.5517/ccdc.csd.cc2gvkvr

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