Title: Perspective: Toward “synthesis by design”: Exploring atomic correlations during inorganic materials synthesis

Abstract

Synthesis of inorganic extended solids is a critical starting point from which real-world functional materials and their consequent technologies originate. However, unlike the rich mechanistic foundation of organic synthesis, with its underlying rules of assembly (e.g., functional groups and their reactivities), the synthesis of inorganic materials lacks an underpinning of such robust organizing principles. In the latter case, any such rules must account for the diversity of chemical species and bonding motifs inherent to inorganic materials and the potential impact of mass transport on kinetics, among other considerations. Without such assembly rules, there is less understanding, less predictive power, and ultimately less control of properties. Despite such hurdles, developing a mechanistic understanding for synthesis of inorganic extended solids would dramatically impact the range of new material discoveries and resulting new functionalities, warranting a broad call to explore what is possible. Here we discuss our recent approaches toward a mechanistic framework for the synthesis of bulk inorganic extended solids, in which either embryonic atomic correlations or fully developed phases in solutions or melts can be identified and tracked during product selection and crystallization. The approach hinges on the application of high-energy x-rays, with their penetrating power and large Q-range, to exploremore » reaction pathways in situ. We illustrate this process using two examples: directed assembly of Zr clusters in aqueous solution and total phase awareness during crystallization from K–Cu–S melts. These examples provide a glimpse of what we see as a larger vision, in which large scale simulations, data-driven science, and in situ studies of atomic correlations combine to accelerate materials discovery and synthesis, based on the assembly of well-defined, prenucleated atomic correlations.« less

Authors:

Soderholm, L.  ^[1];

• Search DOE PAGES for author "Soderholm, L."
• Search DOE PAGES for ORCID "0000-0003-4435-2721"

Mitchell, J. F.  ^[2]

• Search DOE PAGES for author "Mitchell, J. F."
• Search DOE PAGES for ORCID "0000-0002-8416-6424"

---

+ Show Author Affiliations

1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Sciences Division

Publication Date:

Thu May 26 00:00:00 EDT 2016

Research Org.:

Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1352678

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

APL Materials

Additional Journal Information:

Journal Volume: 4; Journal Issue: 5; Journal ID: ISSN 2166-532X

Publisher:

American Institute of Physics (AIP)

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; Materials synthesis; Materials properties; Crystal structure; Solid solutions; X-ray diffraction